Creating a bionic scaffold via light-curing liquid crystal ink to reveal the role of osteoid-like microenvironment in osteogenesis.

Osteoid plays a crucial role in directing cell behavior and osteogenesis through its unique characteristics, including viscoelasticity and liquid crystal (LC) state. Thus, integrating osteoid-like features into 3D printing scaffolds proves to be a promising approach for personalized bone repair. Despite extensive research on viscoelasticity, the role of LC state in bone repair has been largely overlooked due to the scarcity of suitable LC materials. Moreover, the intricate interplay between LC state and viscoelasticity in osteogenesis remains poorly understood. Here, we developed innovative hydrogel scaffolds with osteoid-like LC state and viscoelasticity using digital light processing with a custom LC ink. By utilizing these LC scaffolds as 3D research models, we discovered that LC state mediates high protein clustering to expose accessible RGD motifs to trigger cell-protein interactions and osteogenic differentiation, while viscoelasticity operates via mechanotransduction pathways. Additionally, our investigation revealed a synergistic effect between LC state and viscoelasticity, amplifying cell-protein interactions and osteogenic mechanotransduction processes. Furthermore, the interesting mechanochromic response observed in the LC hydrogel scaffolds suggests their potential application in mechanosensing. Our findings shed light on the mechanisms and synergistic effects of LC state and viscoelasticity in osteoid on osteogenesis, offering valuable insights for the biomimetic design of bone repair scaffolds.

A Wood-Derived Periosteum for Spatiotemporal Drug Release: Boosting Bone Repair through Anisotropic Structure and Multiple Functions.

Existing artificial periostea face many challenges, including difficult-to-replicate anisotropy in mechanics and structure, poor tissue adhesion, and neglected synergistic angiogenesis and osteogenesis. Here, inspired by natural wood (NW), a wood-derived elastic artificial periosteum is developed to mimic the structure and functions of natural periosteum, which combines an elastic wood (EW) skeleton, a polydopamine (PDA) binder layer, and layer-by-layer (LBL) biofunctional layers. Specifically, EW derived from NW is utilized as the anisotropic skeleton of artificial periosteum to guide cell directional behaviors, moreover, it also shows a similar elastic modulus and flexibility to natural periosteum. To further enhance its synergistic angiogenesis and osteogenesis, surface LBL biofunctional layers are designed to serve as spatiotemporal release platforms to achieve sequential and long-term release of pamidronate disodium (PDS) and deferoxamine (DFO), which are pre-encapsulated in chitosan (CS) and hyaluronic acid (HA) solutions, respectively. Furthermore, the combined effect of PDA coating and LBL biofunctional layers enables the periosteum to tightly adhere to damaged bone tissue. More importantly, this novel artificial periosteum can boost angiogenesis and bone formation in vitro and in vivo. This study opens up a new path for biomimetic design of artificial periosteum, and provides a feasible clinical strategy for bone repair.

Chitin whisker/chitosan liquid crystal hydrogel assisted scaffolds with bone-like ECM microenvironment for bone regeneration.

Natural bone exhibits a complex anisotropic and micro-nano hierarchical structure, more importantly, bone extracellular matrix (ECM) presents liquid crystal (LC) phase and viscoelastic characteristics, providing a unique microenvironment for guiding cell behavior and regulating osteogenesis. However, in bone tissue engineering scaffolds, the construction of bone-like ECM microenvironment with exquisite microstructure is still a great challenge. Here, we developed a novel polysaccharide LC hydrogel supported 3D printed poly(l-lactide) (PLLA) scaffold with bone-like ECM microenvironment and micro-nano aligned structure. First, we prepared a chitin whisker/chitosan polysaccharide LC precursor, and then infuse it into the pores of 3D printed PLLA scaffold, which was previously surface modified with a polydopamine layer. Next, the LC precursor was chemical cross-linked by genipin to form a hydrogel network with bone-like ECM viscoelasticity and LC phase in the scaffold. Subsequently, we performed directional freeze-casting on the composite scaffold to create oriented channels in the LC hydrogel. Finally, we soaked the composite scaffold in phytic acid to further physical cross-link the LC hydrogel through electrostatic interactions and impart antibacterial effects to the scaffold. The resultant biomimetic scaffold displays osteogenic activity, vascularization ability and antibacterial effect, and is expected to be a promising candidate for bone repair.

Succinylated chitosan derivative restore HUVEC cells function damaged by TNF-α and high glucose in vitro and enhanced wound healing.

The inflammation of chronic wounds plays a key hindering role in the wound healing process. Slowing down the inflammatory response is significant for the repair of chronic wounds. Studies have revealed that succinate can inactivate gastrin D (GSDMD) and prevent cell pyroptosis. Chitosan has anti-inflammatory properties and is commonly used as wound healing material. Therefore, we used succinic anhydride to modify chitosan and found that N-succinylated chitosan (NSC) was more effective in inhibiting inflammation. The results showed that the stimulation of TNF-α and high glucose induces overexpression of capase-1 and TNF-α in human umbilical vein endothelial cells (HUVEC), and down-expression of CD31. However, the expression of capase-1 and TNF-α decreased, while the expression of CD31, VEGF and IL-10 was up-regulated significantly in dysfunctional HUVEC cells after treated by NSC. Moreover, NSC can speed wound healing, histological examination results showed that wounds treated with NSC exhibited faster epithelial tissue regeneration and thicker collagen deposition. Overall, this study results suggested that NSC has the function of restoring the physiological functions of dysfunctional HUVEC cells induced by high glucose and TNF-α, and can accelerate wound healing, indicating that NSC has good potential to be applied in inflammatory chronic wounds such as diabetic foot.

Chitin nanocrystals stabilized liquid metal for highly stretchable and anti-freeze hydrogels as flexible strain sensor.

Conductive hydrogels show extensive applications in flexible electronics and biomedical areas, but it is a challenge to simultaneously achieve high mechanical properties, satisfied electrical conductivity, good biocompatibility, self-recovery and anti-freezing properties through a simple preparation method. Herein, chitin nanocrystals (ChNCs) were employed to encapsulate liquid metal nanoparticles (LMNPs) to ensure the dispersion stability of LMNPs in a hydrogel system composed of polyacrylamide (PAM) and polyvinyl alcohol (PVA). The synergistic effect of ChNCs-stabilized LMNPs imparts remarkable conductivity to the hydrogel, making it an effective strain sensor for human motion. With 1 % LMNPs, the composite hydrogel stretches up to 2100 %, showing excellent stretchability. Under 10 cycles of 200 % strain, hysteresis loop curves overlap, indicating outstanding fatigue resistance. The hydrogel exhibits remarkable self-recovery, enduring 1400 % deformation without rupture. In addition, its effective antifreeze properties result from immersion in a glycerol-water solvent. Even at -20 °C and 60 °C, the hydrogel maintains stable, reproducible resistance changes at 150 % tensile strain. Therefore, the high-performance conductive hydrogel containing ChNCs stabilized LM has promising applications in flexible wearable sensing devices.

3D Printing Drug-Free Scaffold with Triple-Effect Combination Induced by Copper-Doped Layered Double Hydroxides for the Treatment of Bone Defects.

Tissue-engineered poly(l-lactide) (PLLA) scaffolds have been widely used to treat bone defects; however, poor biological activities have always been key challenges for its further application. To address this issue, introducing bioactive drugs or factors is the most commonly used method, but there are often many problems such as high cost, uncontrollable and monotonous drug activity, and poor bioavailability. Here, a drug-free 3D printing PLLA scaffold with a triple-effect combination induced by surface-modified copper-doped layered double hydroxides (Cu-LDHs) is proposed. In the early stage of scaffold implantation, Cu-LDHs exert a photothermal therapy (PTT) effect to generate high temperature to effectively prevent bacterial infection. In the later stage, Cu-LDHs can further have a mild hyperthermia (MHT) effect to stimulate angiogenesis and osteogenic differentiation, demonstrating excellent vascularization and osteogenic activity. More importantly, with the degradation of Cu-LDHs, the released Cu2+ and Mg2+ provide an ion microenvironment effect and further synergize with the MHT effect to stimulate angiogenesis and osteogenic differentiation, thus more effectively promoting the healing of bone tissue. This triple-effect combined scaffold exhibits outstanding antibacterial, osteogenic, and angiogenic activities, as well as the advantages of low cost, convenient procedure, and long-term efficacy, and is expected to provide a promising strategy for clinical repair of bone defects.

Flexible Hybrid Wearable Sensors for Pressure and Thermal Sensing Based on a Double-Network Hydrogel.

Flexible sensors have attracted great attention due to their wide applications in various fields such as motion monitoring and medical health. It is reasonable to develop a sensor with good flexibility, sensitivity, and biocompatibility for wearable device applications. In this study, a double-network hydrogel was obtained by blending poly(vinyl alcohol) (PVA) with poly(ethylene glycol) diacrylate (PEGDA), which combines the flexibility of the PVA network and the fast photocuring ability of PEGDA. Subsequently, polydopamine-coated carbon nanotubes were used as conductive fillers of the PVA-PEG hydrogel matrix to prepare a flexible sensor that exhibits an effective mechanical response and significant stability in mechanics and conductivity. More importantly, the resistance of the sensor is very sensitive to pressure and thermal changes due to the optimized conductive network in the hydrogel. A motion monitoring test showed that the flexible sensor not only responds quickly to the motion of different joints but also keeps the output signal stable after many cycles. In addition, the excellent cell affinity of the hybrid hydrogel also encourages its application in health monitoring and motion sensors.

Highly anisotropic and elastic cellulosic scaffold guiding cell orientation and osteogenic differentiation via topological and mechanical cues.

Inspired by the similarity of anisotropic channels in wood to the canals of bone, the elastic wood-derived (EW) scaffolds with anisotropic channels were prepared via simple delignification treatment of natural wood (NW). We hypothesize that the degree of delignification will lead to differences in mechanical properties of scaffolds, which in turn directly affect the behaviors and fate of stem cells. The delignification process did not destroy the anisotropic channel structure of the scaffolds, but endowed the scaffolds with good elasticity and rapid stress relaxation. Interestingly, the micron-scale anisotropic channels of the scaffolds can highly promote the polarization of cells along the direction of channels. We also found that the alkaline phosphatase of EW scaffold can reach to about 13.1 U/gprot, which was about double that of NW scaffold. Moreover, the longer the delignification time, the better the osteogenic activity of the EW scaffolds. We further hypothesize that the osteogenic activity of scaffolds is related to the stress relaxation properties. The immunofluorescence staining showed that when the stress relaxation time of scaffold was shortened to about 10 s, the nuclear ratio of YAP of scaffold increased to 0.22, which well supports our hypothesis.

Non-spherical assemblies of chitin nanocrystals by drop impact assembly.

Preparing complex non-spherical assemblies of elongated nanoparticles and exploring their topological conformations is a challenge due to liquid crystals' mobility and elastic distortion. Here, we fabricated a variety of non-spherical liquid crystal assemblies of chitin nanocrystals (ChNCs) in a coagulation bath containing sodium triphosphate (STP) by drop impact assembly method, and the forming mechanism and internal topology were systematically investigated. The collection height, ChNCs concentration, and STP concentration have significant influence on the shape and size of the assembled structures. Long-range ordered structures and long-lived topological textures of the ChNCs liquid crystal can be obtained since a molecular interaction of hydrogen bonding and electrostatic attractions between ChNCs and STP occur during the impact assembly. Rheological and kinetic analysis suggested the shear thinning behavior of the ChNCs liquid crystals and the rapid gelation phenomenon of ChNCs induced by STP. Morphology results showed that the rod-like ChNCs in the non-spherical assemblies were orderly and closely arranged with periodic repetition and layered structure. The non-spherical assemblies of ChNCs liquid crystals can be used as carriers of carbon nanotubes, magnetic Fe3O4 nanoparticles, synthesized polymers, and anticancer drugs for functional composite applications. The drop impact assembly method of ChNCs liquid crystal structure is highly controllable on the composition, morphology, and function, which shows promising applications in energy, environmental-friendly, and bioactive materials.

Preparation of chitin/MXene/poly(L-arginine) composite aerogel spheres for specific adsorption of bilirubin.

Currently, hemoperfusion is clinically the most rapid and effective treatment for removing toxins from the blood. The core of hemoperfusion is the sorbent inside the hemoperfusion device. Due to the complex composition of the blood, adsorbents tend to adsorb substances such as proteins in the blood (non-specific adsorption) while adsorbing toxins. Hyperbilirubinemia is caused by excessive levels of bilirubin in the human blood, causing irreversible damage to the patient's brain and nervous system, and even leading to death. High adsorption and high biocompatibility adsorbents with specific bilirubin adsorption are urgently needed to treat hyperbilirubinemia. Herein, poly(L-arginine) (PLA) which can specifically adsorb bilirubin, was introduced into chitin/MXene (Ch/MX) composite aerogel spheres. Ch/MX/PLA prepared by supercritical CO2 technology had higher mechanical properties than Ch/MX and can withstand 50,000 times its own weight. The in vitro simulated hemoperfusion test showed that the adsorption capacity of Ch/MX/PLA was as high as 596.31 mg/g, which was 15.38 % higher than that of Ch/MX. Binary and ternary competitive adsorption tests showed that Ch/MX/PLA also had good adsorption capacity in the presence of a variety of interfering molecules. In addition, hemolysis rate testing and CCK-8 testing confirmed that Ch/MX/PLA had better biocompatibility and hemocompatibility. Ch/MX/PLA can meet the required properties of clinical hemoperfusion sorbents and has the ability to produce mass production. It has good application potential in the clinical treatment of hyperbilirubinemia.

Modulating of Bouligand Structure and Chirality Constructed Bionically Based on the Self-Assembly of Chitin Whiskers.

Chitin can self-assemble into a liquid crystal phase with supramolecular chirality and Bouligand structure, which is widely found in the exoskeletons of arthropods. However, bionically replicating this structure via the self-assembly of chitin whiskers (CHWs) is still a challenge. Here, the effects of several internal and external parameters on the self-assembly of CHWs were revealed based on liquid crystal phase, chirality, Bouligand structure, and rheological properties. The formation of chiral liquid crystal phase and Bouligand structure largely depends on the concentration of CHWs and, meanwhile, is affected by the aspect ratio and zeta potential of CHWs and the self-assembly time. Impressively, introducing electrolytes and changing pH significantly affect the thickness of the electrical double layer, thereby also affecting the self-assembly of CHWs. This study offers a comprehensive understanding of CHWs' self-assembly process, which is beneficial for the bionic design of new nature-inspired functional materials with chiral characteristic and Bouligand structure.

3D light-curing printing to construct versatile octopus-bionic patches.

Reliable, fast and switchable gluing modes are critically important in medical adhesives and intelligent climbing robot applications. The octopus-bionic patch has attracted the attention of many scholars. The suction cup structure of the octopus achieves adhesion through differential pressure, showing strong adhesion in both dry and wet environments. However, the construction of the octopus-bionic patch remains limited in terms of adaptability, personalization and mass production. Herein, a composite hydrogel consisting of gelatin methacryloyl (GelMA), polyethylene glycol diacrylate (PEGDA) and acrylamide (AAM) was developed, and a structure mimicking the octopus sucker was constructed by digital light processing (DLP). The obtained octopus-bionic patch has strong adhesion, good biocompatibility and multi-functionality. Compared with the template method in most studies, the octopus-bionic patch constructed by the DLP printing method has the advantages of customizability and low cost. In addition, the DLP printing method endows the patch surface with an octopus-like groove structure for a better bionic effect.

Highly Elastic and Anisotropic Wood-Derived Composite Scaffold with Antibacterial and Angiogenic Activities for Bone Repair.

Scaffold-based tissue engineering is a promising strategy to address the rapidly growing demand for bone implants, but developing scaffolds with bone extracellular matrix-like structures, suitable mechanical properties, and multiple biological activities remains a huge challenge. Here, it is aimed to develop a wood-derived composite scaffold with an anisotropic porous structure, high elasticity, and good antibacterial, osteogenic, and angiogenic activities. First, natural wood is treated with an alkaline solution to obtain a wood-derived scaffold with an oriented cellulose skeleton and high elasticity, which can not only simulate collagen fiber skeleton in bone tissue but also greatly improve the convenience of clinical implantation. Subsequently, chitosan quaternary ammonium salt (CQS) and dimethyloxalylglycine (DMOG) are further modified on the wood-derived elastic scaffold through a polydopamine layer. Among them, CQS endows the scaffold with good antibacterial activity, while DMOG significantly improves the scaffold's osteogenic and angiogenic activities. Interestingly, the mechanical characteristics of the scaffolds and the modified DMOG can synergistically enhance the expression of yes-associated protein/transcriptional co-activator with PDZ binding motif signaling pathway, thereby effectively promoting osteogenic differentiation. Therefore, this wood-derived composite scaffold is expected to have potential application in the treatment of bone defects.

Microencapsulated phase change material with chitin nanocrystals stabilized Pickering emulsion for thermal energy storage.

The leakage during the phase change process and low thermal conductivity of PCMs limit their application area. In this study, Pickering emulsion stabilized with chitin nanocrystals (ChNCs) was used to prepare paraffin wax (PW) microcapsules by forming a dense melamine-formaldehyde resin shell on the surface of droplets. The PW microcapsules were then loaded into the metal foam to endow high thermal conductivity to the composite. The PW emulsions could be formed at low concentrations of ChNCs (0.3 wt%), and the PW microcapsules exhibits a favorable thermal cycling stability and a satisfactory latent heat-storage capacity over 170 J/g. Most importantly, the encapsulation of the polymer shell not only endows the microcapsules with high encapsulation efficiency of 98.8 %, non-leakage properties under prolonged high temperature conditions, but also with high flame retardancy. In addition, the composite of PW microcapsules/copper foam shows satisfactory performance in terms of thermal conductivity, thermal storage capacity and thermal reliability, which can be used for effective temperature regulation of heat generating materials. This study provides new design strategy of natural and sustainable nanomaterials stabilized PCMs, which shows promising application in the field of energy management and thermal equipment temperature regulation.

Bone ECM-inspired biomineralization chitin whisker liquid crystal hydrogels for bone regeneration.

As a particular cell niche, natural bone extracellular matrix (ECM) is an organic-inorganic composite material formed by mineralization of liquid crystal (LC) collagen fiber network. However, designing bone repair materials that highly imitate the LC characteristic and composite components of natural bone ECM is a great challenge. Here, we report a novel kind of bone ECM-inspired biomineralization chitin whisker LC hydrogels. First, photocurable chitin whisker LC hydrogels with bone ECM-like chiral nematic LC state and viscoelasticity are created. Next, biomineralization, guided by LC hydrogels, is carried out to truly mimic the mineralization process of natural bone, so as to obtain the organic-inorganic composite materials with bone ECM-like microenvironment. The chitin whisker LC hydrogels exhibit superior biomineralization, protein adsorption and osteogenesis ability, more importantly, LC hydrogel with negatively charged -COOH groups is more conducive to biomineralization and shows more desirable osteogenic activity than that with positively charged -NH2 groups. Notably, compared with the pristine LC hydrogels, the biomineralization LC hydrogels display more favorable osteogenesis ability due to their bone ECM-like LC texture and bone-like hydroxyapatite. This study opens an avenue toward the design of bone ECM-inspired biomineralization chitin whisker LC hydrogels for bone regeneration.

Photocurable liquid crystal hydrogels with different chargeability and tunable viscoelasticity based on chitin whiskers.

We develop a kind of photocurable liquid crystal hydrogels with bone extracellular matrix (ECM)-like liquid crystal state and viscoelasticity, as well as different chargeability. First, positively charged chitin whiskers (CHWs) and negatively charged maleic anhydride chitin whiskers (mCHWs) were prepared, which further self-assemble to form chiral nematic liquid crystals under ultrasonic treatment, respectively. Subsequently, poly (ethylene glycol) diacrylate (PEGDA) and photo initiator were added, and then two kinds of liquid crystal hydrogels with bone ECM-like viscoelasticity and different chargeability were prepared under ultraviolet (UV) irradiation. Benefiting from the bone ECM-like liquid crystal state and viscoelasticity, the prepared liquid crystal hydrogels exhibit remarkable cell affinity and osteogenic ability. Moreover, the liquid crystal hydrogel with negatively charged mCHWs is more favorable for cell adhesion, spreading and osteogenic differentiation than that with positively charged CHWs. This work provides a promising strategy to prepare the hydrogels with bone ECM-like liquid crystal properties and viscoelasticity for bone repair.

Bone ECM-like 3D Printing Scaffold with Liquid Crystalline and Viscoelastic Microenvironment for Bone Regeneration.

Implanting a 3D printing scaffold is an effective therapeutic strategy for personalized bone repair. As the key factor for the success of bone tissue engineering, the scaffold should provide an appropriate bone regeneration microenvironment and excellent mechanical properties. In fact, the most ideal osteogenic microenvironment is undoubtedly provided by natural bone extracellular matrix (ECM), which exhibits liquid crystalline and viscoelastic characteristics. However, mimicking a bone ECM-like microenvironment in a 3D structure with outstanding mechanical properties is a huge challenge. Herein, we develop a facile approach to fabricate a bionic scaffold perfectly combining bone ECM-like microenvironment and robust mechanical properties. Creatively, 3D printing a poly(l-lactide) (PLLA) scaffold was effectively strengthened via layer-by-layer electrostatic self-assembly of chitin whiskers. More importantly, a kind of chitin whisker/chitosan composite hydrogel with bone ECM-like liquid crystalline state and viscoelasticity was infused into the robust PLLA scaffold to build the bone ECM-like microenvironment in 3D structure, thus highly promoting bone regeneration. Moreover, deferoxamine, an angiogenic factor, was encapsulated in the composite hydrogel and sustainably released, playing a long-term role in angiogenesis and thereby further promoting osteogenesis. This scaffold with bone ECM-like microenvironment and excellent mechanical properties can be considered as an effective implantation for bone repair.

Drug-Loaded and Anisotropic Wood-Derived Hydrogel Periosteum with Super Antibacterial, Anti-Inflammatory, and Osteogenic Activities.

Current artificial periostea mainly focus on osteogenic activity but overlook structural and mechanical anisotropy, as well as the importance of antibacterial and anti-inflammatory properties. Here, inspired by the anisotropic structure of wood, the delignified wood (named white wood, WW) with a porous and highly oriented cellulose fiber skeleton was obtained, which was further filled with polyvinyl alcohol (PVA) hydrogel loaded with curcumin (Cur) and phytic acid (PA). The prepared wood-derived hydrogel composite membranes can not only exhibit an obvious anisotropic structure and good mechanical properties but also sustainably release loaded drugs to obtain long-term biological activities. Creatively, PA can effectively improve the bioavailability of Cur; more importantly, Cur and PA play an obvious synergistic effect in antibacterial, anti-inflammatory, and osteogenic activities. Compared with the wood-derived hydrogel composite membranes without drug loading, as well as loaded with Cur or PA only, these loaded with Cur and PA are significantly more conducive to inhibiting the growth of bacteria and inflammatory response and facilitating the adhesion, proliferation, and osteogenic differentiation of bone marrow mesenchymal stem cells. This kind of anisotropic wood-derived hydrogel composite membrane with fantastic antibacterial, anti-inflammatory, and osteogenic activities is expected to be ideal artificial periostea.

Carbon Nanotube Ink Dispersed by Chitin Nanocrystals for Thermoelectric Converter for Self-Powering Multifunctional Wearable Electronics.

The screen-printing process of conductive ink can realize simple and large-scale manufacture of micro/nano patterns for producing wearable electronic products. Herein, chitin nanocrystals (ChNCs) are used as a dispersant for the preparation of multiwalled carbon nanotube (MWCNT) ink with high viscosity and uniformity by ultrasound treatment. ChNCs can interact with MWCNT in noncovalent ways, including π-π and hydrophobic interactions. ChNCs/MWCNT (CCNT) ink does not aggregate even after standing for 3 months with a maximum MWCNT concentration of 33 mg mL-1 and dispersion efficiency of 91.1%. Using CCNT ink, a paper-based thermoelectric generator (TEG) is manufactured by screen-printing technology. With good thermoelectric and strain sensing properties, CCNT coated paper can stably collect human energy at room temperature to realize self-powering. The CCNT coated paper-based TEG can convert thermal voltage signals into musical notes, monitor the changes in human behavior and respiratory rate, and monitor joint movements. Moreover, CCNT coated paper has no cytotoxicity by CCK-8 and live/dead staining. This work puts forward a strategy of green preparation of MWCNT-based ink by adding renewable chitin, which opens up a new way to apply MWCNT-based ink in self-powering wearable multifunctional sensors.

Dual-Cross-linked Liquid Crystal Hydrogels with Controllable Viscoelasticity for Regulating Cell Behaviors.

The liquid crystal properties and viscoelasticity of the natural bone extracellular matrix (ECM) play a decisive role in guiding cell behavior, conducting cell signals, and regulating mineralization. Here, we develop a facile approach for preparing a novel polysaccharide hydrogel with liquid crystal properties and viscoelasticity similar to those of natural bone ECM. First, a series of chitin whisker/chitosan (CHW/CS) hydrogels were prepared by chemical cross-linking with genipin, in which CHW can self-assemble to form cholesteric liquid crystals under ultrasonic treatment and CS chains can enter into the gaps between the helical layers of the CHW cholesteric liquid crystal phase to endow morphological stability and good mechanical properties. Subsequently, the obtained chemically cross-linked liquid crystal hydrogels were immersed into the desired concentration of the NaCl solution to form physical cross-linking. Due to the Hofmeister effect, the as-prepared dual-cross-linked liquid crystal hydrogels showed an enhanced modulus, viscoelasticity similar to that of natural ECM with relatively fast stress relaxation behavior, and fold surface morphology. Compared to both CHW/CS hydrogels without liquid crystal properties and CHW/CS liquid crystal hydrogels without further physical cross-linking, the dual-cross-linked CHW/CS liquid crystal hydrogels are more favorable for the adhesion, proliferation, and osteogenic differentiation of bone marrow mesenchymal stem cells. This approach could inspire the design of hydrogels mimicking the liquid crystal properties and viscoelasticity of natural bone ECM for bone repair.