Biotropic liquid crystal phase transformations in cellulose-producing bacterial communities.

Biological functionality is often enabled by a fascinating variety of physical phenomena that emerge from orientational order of building blocks, a defining property of nematic liquid crystals that is also pervasive in nature. Out-of-equilibrium, "living" analogs of these technological materials are found in biological embodiments ranging from myelin sheath of neurons to extracellular matrices of bacterial biofilms and cuticles of beetles. However, physical underpinnings behind manifestations of orientational order in biological systems often remain unexplored. For example, while nematiclike birefringent domains of biofilms are found in many bacterial systems, the physics behind their formation is rarely known. Here, using cellulose-synthesizing Acetobacter xylinum bacteria, we reveal how biological activity leads to orientational ordering in fluid and gel analogs of these soft matter systems, both in water and on solid agar, with a topological defect found between the domains. Furthermore, the nutrient feeding direction plays a role like that of rubbing of confining surfaces in conventional liquid crystals, turning polydomain organization within the biofilms into a birefringent monocrystal-like order of both the extracellular matrix and the rod-like bacteria within it. We probe evolution of scalar orientational order parameters of cellulose nanofibers and bacteria associated with fluid-gel and isotropic-nematic transformations, showing how highly ordered active nematic fluids and gels evolve with time during biological-activity-driven, disorder-order transformation. With fluid and soft-gel nematics observed in a certain range of biological activity, this mesophase-exhibiting system is dubbed "biotropic," analogously to thermotropic nematics that exhibit solely orientational order within a temperature range, promising technological and fundamental-science applications.

Acoustic force spectroscopy reveals subtle differences in cellulose unbinding behavior of carbohydrate-binding modules.

Protein adsorption to solid carbohydrate interfaces is critical to many biological processes, particularly in biomass deconstruction. To engineer more-efficient enzymes for biomass deconstruction into sugars, it is necessary to characterize the complex protein-carbohydrate interfacial interactions. A carbohydrate-binding module (CBM) is often associated with microbial surface-tethered cellulosomes or secreted cellulase enzymes to enhance substrate accessibility. However, it is not well known how CBMs recognize, bind, and dissociate from polysaccharides to facilitate efficient cellulolytic activity, due to the lack of mechanistic understanding and a suitable toolkit to study CBM-substrate interactions. Our work outlines a general approach to study the unbinding behavior of CBMs from polysaccharide surfaces using a highly multiplexed single-molecule force spectroscopy assay. Here, we apply acoustic force spectroscopy (AFS) to probe a Clostridium thermocellum cellulosomal scaffoldin protein (CBM3a) and measure its dissociation from nanocellulose surfaces at physiologically relevant, low force loading rates. An automated microfluidic setup and method for uniform deposition of insoluble polysaccharides on the AFS chip surfaces are demonstrated. The rupture forces of wild-type CBM3a, and its Y67A mutant, unbinding from nanocellulose surfaces suggests distinct multimodal CBM binding conformations, with structural mechanisms further explored using molecular dynamics simulations. Applying classical dynamic force spectroscopy theory, the single-molecule unbinding rate at zero force is extrapolated and found to agree with bulk equilibrium unbinding rates estimated independently using quartz crystal microbalance with dissipation monitoring. However, our results also highlight critical limitations of applying classical theory to explain the highly multivalent binding interactions for cellulose-CBM bond rupture forces exceeding 15 pN.

Bacterial nanocellulose: A versatile biopolymer production using a cost-effective wooden disc based rotary reactor.

Bacterial nanocellulose (BNC) has various unique qualities, including high mechanical strength, crystallinity, and high water-holding capacity, which makes it appropriate for a wide range of industrial applications. But its lower yield coupled with its high production cost creates a barrier to its usage. In this study, we have demonstrated the better yield of BNC from an indigenous strain Komagataeibacter rhaeticus MCC-0157 using a rotary disc bioreactor (RDB) having a wooden disc. The RDB was optimized based on the type of disc material, distance between the disc, and rotation speed to get the highest yield of 13.0 g/L dry material using Hestrin-Schramm (H-S) medium. Further, the bioreactor was compared for the BNC production using reported medium, which is used for static condition; the RDB showed up to fivefold increase in comparison with the static condition reported. Komagataeibacter rhaeticus MCC-0157 was previously reported to be one of the highest BNC producing stains, with 8.37 g/L of dry yield in static condition in 15 days incubation. The designed RDB demonstrated 13.0 g/L dry yield of BNC in just 5 days. Other characteristics of BNC remain same as compared with static BNC production, although the difference in the crystallinity index was observed in RDB (84.44%) in comparison with static (89.74%). For the first time, wooden disc was used for rotary bioreactor approach, which demonstrated higher yield of BNC in lesser time and can be further used for sustainable production of BNC at the industrial level.

Silver-nanoparticle-modified nanocellulose synthesized by pyroligneous acid: cytotoxicity towards HaCat cells.

In the present study, pyroligneous acid, also known as wood vinegar, has been employed as reducing and stabilizing agent in the synthesis of silver nanoparticles (AgNPs) anchored on nanocellulose (NC). The idea is to confer the latter bactericidal properties for its typical uses such as in cosmetics and food-packing. It has been demonstrated that AgNPs can be directly produced onto NC in one-pot fashion while dramatically enhancing the kinetics of AgNPs synthesis (2 h for reaction completion) in comparison to the NC-less counterpart (10 days for reaction completion). Furthermore, NC allowed for a narrower size distribution of AgNPs. NC-supported and non-supported AgNPs had sizes of 5.1 ± 1.6 nm and 16.7 ± 4.62 nm, respectively. Immortalized human keratinocytes (HaCat) cells were then employed as model to evaluate the cytotoxicity of the AgNPs-NC compound. The latter was found not to impact cell proliferation at any formulation, while decreasing the viability by only 6.8% after 72 h. This study contributes to the development of more environmentally benign routes to produce nanomaterials and to the understanding of their impact on cells.

Transparent Multilayer Acrylic Composites Reinforced with Poly(Acrylated Urethane) Filled Low Grammage Bacterial Cellulose Nanopaper.

Cellulose nanopaper is a material structure that possesses high mechanical performance and is widely regarded as a promising 2D reinforcement for polymer matrix composites. This work explores the use of low grammage bacterial cellulose (BC) nanopaper as reinforcement for poly(acrylated urethane) interlayer adhesive to increase the impact performance of multilayer acrylic composites. The BC nanopaper is impregnated with an acrylated urethane resin and laminated between acrylic sheets to create BC/acrylic composites consisting of one, three, and five layers of BC nanopaper-reinforced poly(acrylated urethane) interlayer adhesive(s). Both the poly(acrylated urethane)-filled BC nanopaper interlayer adhesive and the resulting laminated acrylic composites are optically transparent. The incorporation of BC nanopaper into the poly(acrylated urethane) interlayer adhesive improves the tensile modulus by eightfold and the single-edge notched fracture toughness by 60% compared to neat poly(acrylated urethane). It is also found that using poly(acrylated urethane)-filled BC nanopaper interlayer adhesive proves beneficial to the impact properties of the resulting laminated acrylic composites. In Charpy impact testing, the impact strength of the multilayer acrylic composites increases by up to 130% compared to the "gold-standard" impact-modified monolithic acrylic, with a BC loading of only 1.6 wt%.

Cellulose-alginate hydrogels and their nanocomposites for water remediation and biomedical applications.

In the last decade, both cellulose and alginate polysaccharides have been extensively utilized for the synthesis of biocompatible hydrogels because of their alluring characteristics like low cost, biodegradability, hydrophilicity, biodegradability, ease of availability and non-toxicity. The presence of abundant hydrophilic functional groups (like carboxyl and hydroxyl) on the surface of cellulose and alginate or their derivatives makes these materials promising candidates for the preparation of hydrogels with appealing structures and characteristics, leading to growing research in water treatment and biomedical fields. These two polysaccharides are typically blended together to improve hydrogels' desired qualities (mechanical strength, adsorption properties, cellulose/alginate yield). So, keeping in view their extensive applicability, in the present review article, recent advances in the development of cellulose/nanocellulose-alginate-based hydrogels and their relevance in water treatment (adsorption of dyes, heavy metals, etc.) and biomedical field (wound healing, tissue engineering, drug delivery) has been reviewed. Further, impact of other inorganic/organic additives in cellulose/nanocellulose-alginate-based hydrogels properties like contaminants adsorption, drug delivery, tissue engineering, etc., has also been studied. Moreover, the current difficulties and future prospects of nanocellulose-alginate-based hydrogels regarding their water purification and biomedical applications are also discussed at the end.

Bacterial nanocellulose-clay film as an eco-friendly sorbent for superior pollutants removal from aqueous solutions.

The persistent water treatment and separation challenge necessitates innovative and sustainable advances to tackle conventional and emerging contaminants in the aquatic environment effectively. Therefore, a unique three-dimensional (3D) network composite film (BNC-KC) comprised of bacterial nanocellulose (BNC) incorporated nano-kaolinite clay particles (KC) was successfully synthesized via an in-situ approach. The microscopic characterization of BNC-KC revealed an effective integration of KC within the 3D matrix of BNC. The investigated mechanical properties of BNC-KC demonstrated a better performance compared to BNC. Thereafter, the sorption performance of BNC-KC films towards basic blue 9 dye (Bb9) and norfloxacin (NFX) antibiotic from water was investigated. The maximum sorption capacities of BNC-KC for Bb9 and NFX were 127.64 and 101.68 mg/g, respectively. Mechanistic studies showed that electrostatic interactions, multi-layered sorption, and 3D structure are pivotal in the NFX/Bb9 sorption process. The intricate architecture of BNC-KC effectively traps molecules within the interlayer spaces, significantly increasing sorption efficiency. The distinctive structural configuration of BNC-KC films effectively addressed the challenges of post-water treatment separation while concurrently mitigating waste generation. The environmental evaluation, engineering, and economic feasibility of BNC-KC are also discussed. The cost estimation assessment of BNC-KC revealed the potential to remove NFX and Bb9 from water at an economically viable cost.

A novel cost-effective methodology for the screening of nanocellulose producing micro-organisms.

In this paper, the work has been done to develop a cost-effective methodology, for the isolation of the potential producer of bacterial nanocellulose. No report is available in the literature, on the use of gram flour and table sugar for the screening of nanocellulose-producing isolates. Since commercially used, Hestrin-Schramm medium is expensive for the isolation of nanocellulose-producing micro-organisms, the possibility of using gram flour-table sugar medium was investigated in this work. Qualitative screening of micro-organisms was done using cost-effective medium, i.e., gram flour-table sugar medium. Qualitative analysis of various nanocellulose-producing bacteria depicted that cellulose layer production occurred on both HS medium and gram flour-table sugar medium. The yield of nanocellulose was also better on air-liquid surface in case of gram flour-table sugar medium as compared to HS medium. 16S rRNA was used for molecular characterization of bacterial strain and the best nanocellulose producer was identified as Novacetimonas hansenii BMK-3_NC240423 (isolated from rotten banana). FTIR and FE-SEM studies of nanocellulose pellicle produced on HS medium and gram flour-table sugar medium demonstrated equivalent structural, morphological, and chemical properties. The cost of newly designed medium (0.01967 $/L) is nearly 90 times lower than the Hestrin-Schramm medium (1.748 $/L), which makes the screening of nanocellulose producers very cost-effective. A strategy of using gram flour extract-table sugar medium for the screening of nanocellulose-producing micro-organisms is a novel approach, which will drastically reduce the screening associated cost of cellulose-producing micro-organisms and also motivate the researchers/industries for comprehensive screening programme for getting high cellulose-producing microbes.

Nanocellulose-Based Materials for Water Pollutant Removal: A Review.

Cellulose in the nano regime, defined as nanocellulose, has been intensively used for water treatment. Nanocellulose can be produced in various forms, including colloidal, water redispersible powders, films, membranes, papers, hydrogels/aerogels, and three-dimensional (3D) objects. They were reported for the removal of water contaminants, e.g., heavy metals, dyes, drugs, pesticides, pharmaceuticals, microbial cells, and other pollutants from water systems. This review summarized the recent technologies for water treatment using nanocellulose-based materials. A scientometric analysis of the topic was also included. Cellulose-based materials enable the removal of water contaminants, and salts offer advanced technologies for water desalination. They are widely used as substrates, adsorbents, and catalysts. They were applied for pollutant removal via several methods such as adsorption, filtration, disinfection, coagulation/flocculation, chemical precipitation, sedimentation, filtration (e.g., ultrafiltration (UF), nanofiltration (NF)), electrofiltration (electrodialysis), ion-exchange, chelation, catalysis, and photocatalysis. Processing cellulose into commercial products enables the wide use of nanocellulose-based materials as adsorbents and catalysts.

Mechanochemical recycling of cellulose multilayer carton packages to produce micro and nanocellulose from the perspective of techno-economic and environmental analysis.

Despite being composed of recyclable materials, the main technological challenge of multilayer carton packs involves the efficient decompatibilization of the cellulosic, polymeric, and metallic phases. Here, a simple two-step mechanochemical process is described that uses only aqueous media and mechanical force to promote phase separation in order to fully recycle multi-layer carton packaging. The first step produces value-added micro- and nanocellulose, while in the second step, aluminum is extracted, forming precipitated aluminum and aluminum oxyhydroxides. Solid polyethylene (PE) remains with a degree of purity defined by the process efficiency. The results show that cellulose is efficiently extracted and converted into micro- and nanocellulose after 15 min of milling. In the second stage, approximately 90% of the aluminum is extracted from the PE after 15 min of milling. Due to the separation and drying medium conditions, the finely divided particles of extracted aluminum also have oxyhydroxides in their composition. It is believed that a passivation layer forms on the metallic aluminum particle. The techno-economic analysis revealed a positive net present value (NPV) of $17.5 million, with a minimum selling price of 1.62 USD/kg of cellulose. The environmental analysis concluded that most of the environmental impact of the process is associated with the entry of carton packages into the system, incorporating a small environmental load related to the industrial process. The results indicate a promising option toward a circular economy and carbon neutrality.

Nanocellulose and its modified forms in the food industry: Applications, safety, and regulatory perspectives.

Nanocellulose (NC), known for its unique properties including high mechanical strength, low density, and extensive surface area, presents significant potential for broad application in the food sector. Through further modification, NC can be enhanced and adapted for various purposes. Applications in the food industry include stabilizing, encapsulating, and packaging material. Additionally, due to its unique characteristics during digestion in the gastrointestinal tract, NC and its derivatives exhibit the potential to be used as health-promotion food ingredients. However, while the safety data on unmodified NC is readily available, the safety of modified forms of NC for use in food remains uncertain. This review offers a comprehensive analysis of recent breakthroughs in NC and its derivatives for innovative food applications. It synthesizes existing research on safety evaluations, with a particular emphasis on the latest findings on toxicity and biocompatibility. Furthermore, the paper outlines the regulatory landscape for NC-based food ingredients and food contact materials in the United States and European Union and provides recommendations to expedite regulatory authorization and commercialization. Ultimately, this work offers valuable insights to promote the sustainable and innovative application of NC compounds in the food sector.

Drug-Loading Content Influences Cellular Uptake of Polymer-Coated Nanocellulose.

While the effects of nanoparticle properties such as shape and size on cellular uptake are widely studied, influences exerted by drug loading have so far been ignored. In this work, nanocellulose (NC) coated by Passerini reaction with poly(2-hydroxy ethyl acrylate) (PHEA-g-NC) was loaded with various amounts of ellipticine (EPT) by electrostatic interactions. The drug-loading content was determined by UV-vis spectroscopy to range between 1.68 and 8.07 wt %. Dynamic light scattering and small-angle neutron scattering revealed an increased dehydration of the polymer shell with increasing drug-loading content, which led to higher protein adsorption and more aggregation. The nanoparticle with the highest drug-loading content, NC-EPT8.0, displayed reduced cellular uptake in U87MG glioma cells and MRC-5 fibroblasts. This also translated into reduced toxicity in these cell lines as well as the breast cancer MCF-7 and the macrophage RAW264.7 cell lines. Additionally, the toxicity in U87MG cancer spheroids was unfavorable. The nanoparticle with the best performance was found to have intermediate drug-loading content where the cellular uptake was adequately high while each nanoparticle was able to deliver a sufficiently toxic amount into the cells. Medium drug loading did not hinder uptake into cells while maintaining sufficiently toxic drug concentrations. It was concluded that while striving for a high drug-loading content is appropriate when designing clinically relevant nanoparticles, it needs to be considered that the drug can cause changes in the physicochemical properties of the nanoparticles that might cause unfavorable effects.

Detection of gases and organic vapors by cellulose-based sensors.

The growing interest in the development of cost-effective, straightforward, and rapid analytical systems has found cellulose-based materials, including cellulose derivatives, cellulose-based gels, nanocellulosic materials, and the corresponding (nano)cellulose-based composites, to be valuable platforms for sensor development. The present work presents recent advances in the development of cellulose-based sensors for the determination of volatile analytes and derivatives of analytical relevance. In particular, strategies described in the literature for the fabrication and modification of cellulose-based substrates with responsive materials are summarized. In addition, selected contributions reported in the field of paper-based volatile sensors are discussed, with a particular emphasis on quick response (QR) code paper-based platforms, intelligent films for food freshness monitoring, and sensor arrays for volatile discrimination purposes. Furthermore, analytical strategies devised for the determination of ionic species by in situ generation of volatile derivatives in both paper-based analytical devices (PADs) and microfluidic PADs will also be described.

Evaporative Dry Powders Derived from Cellulose Nanofiber Organogels to Fully Recover Inherent High Viscosity and High Transparency of Water Dispersion.

Water containing low amounts of cellulose nanofiber (CNF) is widely used as a thickening agent owing to its three unique properties: high transparency, viscosity, and controllable viscosity based on the shear rate. CNF dry powders are used to reduce the transportation and storage costs or expand applications as a thickening agent. Herein, the preparation of CNF dry powders that can be used to obtain redispersions while maintaining the aforementioned properties is reported. In this regard, the dehydration and vaporization procedures for a CNF water dispersion without using additives are discussed. When dry powders are prepared by removing water by boiling, their redispersions do not exhibit all their unique properties because of dense aggregations. However, when their redispersions are vigorously stirred to break the dense aggregations, they become transparent, although they do not recover their initial viscosity. Freeze-dried powders recover all their initial properties after redispersion. Nevertheless, their large volume does not reduce the transportation and storage costs. When the liquid is evaporated from the solvent-exchanged CNF organogels, their redispersions also fully recover all their properties. Furthermore, the evaporative dry powders with dense small volumes and good handling contribute to reducing the transportation and storage costs.

Nanocellulose-based composite aerogels toward the environmental protection: Preparation, modification and applications.

Nanocellulose aerogel has the advantages of porosity, low density and high specific surface area, which can effectively realize the adsorption and treatment of wastewater waste gas. The methods of preparing nanocellulose mainly include mechanical, chemical and biological methods. Nanocellulose is formed into nanocellulose aerogel after gelation, solvent replacement and drying processes. Based on the advantages of easy modification of nanocellulose aerogels, nanocellulose aerogels can be functionalized with conductive fillers, reinforcing fillers and other materials to give nanocellulose aerogels in electrical, mechanical and other properties. Through functionalization, the properties of nanocellulose composite aerogel such as hydrophobicity and adsorption are improved, and the aerogel is endowed with the ability of electrical conductivity and electromagnetic shielding. Through functionalization, the applicability and general applicability of nanocellulose composite aerogel in the field of environmental protection are improved. In this paper, the preparation and functional modification methods of nanocellulose aerogels are reviewed, and the application prospects of nanocellulose composite aerogels in common environmental protection fields such as dye adsorption, heavy metal ion adsorption, gas adsorption, electromagnetic shielding, and oil-water separation are specifically reviewed, and new solutions are proposed.

Valorization of nano-based lignocellulosic derivatives to procure commercially significant value-added products for biomedical applications.

Biowaste, produced from nature, is preferred to be a good source of carbon and ligninolytic machinery for many microorganisms. They are complex biopolymers composed of lignin, cellulose, and hemicellulose traces. This biomass can be depolymerized to its nano-dimensions to gain exceptional properties useful in the field of cosmetics, pharmaceuticals, high-strength materials, etc. Nano-sized biomass derivatives overcome the inherent drawbacks of the parent material and offer promises as a potential material for a wide range of applications with their unique traits such as low-toxicity, biocompatibility, biodegradability and environmentally friendly nature with versatility. This review focuses on the production of value-added products feasible from nanocellulose, nano lignin, and xylan nanoparticles which is quite a novel study of its kind. Dawn of nanotechnology has converted bio waste by-products (hemicellulose and lignin) into useful precursors for many commercial products. Nano-cellulose has been employed in the fields of electronics, cosmetics, drug delivery, scaffolds, fillers, packaging, and engineering structures. Xylan nanoparticles and nano lignin have numerous applications as stabilizers, additives, textiles, adhesives, emulsifiers, and prodrugs for many polyphenols with an encapsulation efficiency of 50%. This study will support the potential development of composites for emerging applications in all aspects of interest and open up novel paths for multifunctional biomaterials in nano-dimensions for cosmetic, drug carrier, and clinical applications.

Potential issues specific to cytotoxicity tests of cellulose nanofibrils.

Cellulose nanofibrils (also called cellulose nanofibers or nanofibrillated cellulose [CNFs]) are novel polymers derived from biomass with excellent physicochemical properties and various potential applications. However, the introduction of such new materials into the market requires thorough safety studies to be conducted. Recently, toxicity testing using cultured cells has attracted attention as a safety assessment that does not rely on experimental animals. This article reviews recent information regarding the cytotoxicity testing of CNFs and highlights the issues relevant to evaluating tests. In the literature, we found that a variety of cell lines and CNF exposure concentrations was evaluated. Furthermore, the results of cytotoxicity results tests differed and were not necessarily consistent. Numerous reports that we examined had not evaluated endotoxin/microbial contamination or the interaction of CNFs with the culture medium used in the tests. The following potential specific issues involved in CNF in vitro testing, were discussed: (1) endotoxin contamination, (2) microbial contamination, (3) adsorption of culture medium components to CNFs, and (4) changes in aggregation/agglomeration and dispersion states of CNFs resulting from culture medium components. In this review, the available measurement methods and solutions for these issues are also discussed. Addressing these points will lead to a better understanding of the cellular effects of CNFs and the development of safer CNFs.

Enhanced High Thermal Conductivity Cellulose Filaments via Hydrodynamic Focusing.

Nanocellulose is regarded as a green and renewable nanomaterial that has attracted increased attention. In this study, we demonstrate that nanocellulose materials can exhibit high thermal conductivity when their nanofibrils are highly aligned and bonded in the form of filaments. The thermal conductivity of individual filaments, consisting of highly aligned cellulose nanofibrils, fabricated by the flow-focusing method is measured in dried condition using a T-type measurement technique. The maximum thermal conductivity of the nanocellulose filaments obtained is 14.5 W/m-K, which is approximately five times higher than those of cellulose nanopaper and cellulose nanocrystals. Structural investigations suggest that the crystallinity of the filament remarkably influence their thermal conductivity. Smaller diameter filaments with higher crystallinity, that is, more internanofibril hydrogen bonds and less intrananofibril disorder, tend to have higher thermal conductivity. Temperature-dependence measurements also reveal that the filaments exhibit phonon transport at effective dimension between 2D and 3D.

Oil-in-Water Pickering Emulsions Stabilized with Nanostructured Biopolymers: A Venue for Templating Bacterial Cellulose.

Pickering emulsions (PEs) differ from conventional emulsions in the use of solid colloidal particles as stabilizing agents instead of traditional amphiphilic molecules. Nanostructured biopolymers (NBs) emerge as a promising alternative for PE stabilization owing to their remarkable biocompatibility, abundant availability, and low cost. To explore this potential, a study is herein presented, in which cellulose nanocrystals (CNCs), both type I and type II allomorphs, and chitin nanocrystals (ChNCs) were used for stabilizing oil-in-water PEs prepared by the use of ultrasound. Sunflower oil was selected as the oil phase as it offers the advantages of being edible, renewable, and inexpensive. By utilizing ζ-potential, static light diffraction, and visual observations, we determined the optimal oil/water ratio for each type of NB to obtain stable emulsions after 14 days. The optimized PEs were used to form bacterial nanocellulose composites through emulsion templating. To our knowledge, this study represents a pioneering work in exploiting oil-in-water PEs for this approach. Additionally, it entails the first utilization of nonmercerized type II CNCs as stabilizers for PEs, while also establishing a direct comparison among the most relevant NBs. The resulting composites exhibited a unique morphology, composed of larger pores compared to standard bacterial nanocellulose aerogels. These findings highlight the notable potential of NBs as stabilizers for PEs and their ability to generate green nanocomposites with tailored properties.

Lignin nanoparticle-decorated nanocellulose cryogels as adsorbents for pharmaceutical pollutants.

Adsorption is a relatively simple wastewater treatment method that has the potential to mitigate the impacts of pharmaceutical pollution. This requires the development of reusable adsorbents that can simultaneously remove pharmaceuticals of varying chemical structure and properties. Here, the adsorption potential of nanostructured wood-based adsorbents towards different pharmaceuticals in a multi-component system was investigated. The adsorbents in the form of macroporous cryogels were prepared by anchoring lignin nanoparticles (LNPs) to the nanocellulose network via electrostatic attraction. The naturally anionic LNPs were anchored to cationic cellulose nanofibrils (cCNF) and the cationic LNPs (cLNPs) were combined with anionic TEMPO-oxidized CNF (TCNF), producing two sets of nanocellulose-based cryogels that also differed in their overall surface charge density. The cryogels, prepared by freeze-drying, showed layered cellulosic sheets randomly decorated with spherical lignin on the surface. They exhibited varying selectivity and efficiency in removing pharmaceuticals with differing aromaticity, polarity and ionic characters. Their adsorption potential was also affected by the type (unmodified or cationic), amount and morphology of the lignin nanomaterials, as well as the pH of the pharmaceutical solution. Overall, the findings revealed that LNPs or cLNPs can act as functionalizing and crosslinking agents to nanocellulose-based cryogels. Despite the decrease in the overall positive surface charge, the addition of LNPs to the cCNF-based cryogels showed enhanced adsorption, not only towards the anionic aromatic pharmaceutical diclofenac but also towards the aromatic cationic metoprolol (MPL) and tramadol (TRA) and neutral aromatic carbamazepine. The addition of cLNPs to TCNF-based cryogels improved the adsorption of MPL and TRA despite the decrease in the net negative surface charge. The improved adsorption was attributed to modes of removal other than electrostatic attraction, and they could be π-π aromatic ring or hydrophobic interactions brought by the addition of LNPs or cLNPs. However, significant improvement was only found if the ratio of LNPs or cLNPs to nanocellulose was 0.6:1 or higher and with spherical lignin nanomaterials. As crosslinking agents, the LNPs or cLNPs affected the rheological behavior of the gels, and increased the firmness and decreased the water holding capacity of the corresponding cryogels. The resistance of the cryogels towards disintegration with exposure to water also improved with crosslinking, which eventually enabled the cryogels, especially the TCNF-based one, to be regenerated and reused for five cycles of adsorption-desorption experiment for the model pharmaceutical MPL. Thus, this study opened new opportunities to utilize LNPs in providing nanocellulose-based adsorbents with additional functional groups, which were otherwise often achieved by rigorous chemical modifications, at the same time, crosslinking the nanocellulose network.