Reducing Dielectric Loss of High-Dielectric-Constant Elastomer via Rigid Short-Chain Crosslinking.

High-dielectric-constant elastomers have broad applications in wearable electronics, which can be achieved by the elastification of relaxor ferroelectric polymers. However, the introduction of soft long chains, with their high mobility under strong electric fields, leads to high dielectric loss. Given the relatively low modulus of relaxor ferroelectric polymers, elastification can be realized by introducing short-chain crosslinkers. In this work, a molecular engineering design is employed, utilizing a rigid short-chain crosslinker to create crosslinks with relaxor ferroelectric polymer, resulting in intrinsic elastomers characterized by a high dielectric constant but low dielectric loss. The obtained intrinsic ferroelectric elastomer possesses a high dielectric constant (35 at 1 kHz and 25 °C) and a low dielectric loss (0.09). Furthermore, this elastomer exhibits stable ferroelectric response and relaxor characteristics even under strains up to 80%. The study supplies a simple but effective method to reduce the dielectric loss of high-dielectric-constant intrinsic elastomers, thereby expanding their application fields in wearable electronics.

Building Ultrastrong, Tough and Biodegradable Thermoplastic Elastomers from Multiblock Copolyesters via a "Reserve-Release" Crystallization Strategy.

Simultaneously attaining high strength and toughness has been a significant challenge in designing thermoplastic elastomers, especially biodegradable ones. In this context, we present a class of biodegradable elastomers based on multiblock copolyesters that afford extraordinary strength, toughness, and low-strain resilience despite expedient chemical synthesis and sample processing. With the incorporation of the semi-crystalline soft block and the judicious selection of block periodicity, the thermoplastic materials feature low quiescent crystallinity ("reserve") albeit with vast potential for strain-induced crystallization ("release"), resulting in their significantly enhanced ultimate strength and energy-dissipating capabilities. Moreover, a breadth of mechanical responses of the materials - from reinforced elastomers to shape-memory materials to toughened thermoplastics - can be achieved by orthogonal variation of segment lengths and ratios. This work and the "reserve-release" crystallization strategy herein highlight the double crystalline multiblock chain architecture as a potential avenue towards reconciling the strength-toughness trade-off in thermoplastic elastomers and can possibly be extended to other biodegradable building blocks to deliver functional materials with diverse mechanical performances.

Recent Advances in Propylene-Based Elastomers Polymerized by Homogeneous Catalysts.

Propylene-based elastomers (PBEs) have received widespread attention and research in recent years due to their structural diversity and excellent properties, and are also an important area for leading chemical companies to compete for layout, but efficient synthesis of PBEs remains challenging. In this paper, we review the development of PBEs and categorize them into three types, grounded in their unique chain structures, including homopolymer propylene-based elastomers (hPBEs), random copolymer propylene-based elastomers (rPBEs), and block copolymer propylene-based elastomers (bPBEs). The successful synthesis of these diverse PBEs is largely credited to the relentless innovative advancements in homogeneous catalysts (metallocene catalysts, constrained geometry catalysts, and non-metallocene catalysts). Consequently, we summarize the catalytic performance of various homogeneous catalysts employed in PBE synthesis and delve into their effect on molecular weight, molecular weight distribution, and chain structures of the resulting PBEs. In the end, based on the current academic research and industrialization status of PBEs, an outlook on potential future research directions for PBEs is provided.

A robust bio-based polyurethane employed as surgical suture with help to promote skin wound healing.

Designing bio-based polyurethane materials with excellent mechanical, biocompatibility, and self-healing properties simultaneously is currently a significant challenge due to the increasing demands for high-performance materials. In this study, we propose an asymmetric backbone strategy utilizing bio-based polycarbonate as the soft segment, equimolar ratios of lysine diisocyanate and isophorone diisocyanate as asymmetric hard segments, and isophorone diamine as the chain extender. The resulting polyurethane elastomers exhibit excellent mechanical properties, including high tensile stress (46.1 MPa), toughness (213.9 MJ/m3), and fracture energy (98.47 kJ/m3). The polyurethane elastomers demonstrate good self-healing and recyclable properties under simple heat treatment. Furthermore, biological experiments confirm the degradability and bio-safety of the bio-based polyurethane elastomers, which have shown potential in accelerating wound healing in mice when used as surgical sutures. These findings highlight the promising prospects of the obtained polyurethane elastomers in various applications, including biomedicine, flexible sensing, and electronic components.

Strong and Healable Elastomers with Photothermal-Stimulus Dynamic Nanonetworks Enabled by Subnano Ultrafine MoO3-x Nanowires.

One-dimensional nanomaterials have become one of the most available nanoreinforcing agents for developing next-generation high-performance functional self-healing composites owing to their unique structural characteristics and surface electron structure. However, nanoscale control, structural regulation, and crystal growth are still enormous challenges in the synthesis of specific one-dimensional nanomaterials. Here, oxygen-defective MoO3-x nanowires with abundant surface dynamic bonding were successfully synthesized as novel nanofillers and photothermal response agents combined with a polyurethane matrix to construct composite elastomers, thus achieving mechanically enhanced and self-healing properties. Benefiting from the surface plasmon resonance of the MoO3-x nanowires and interfacial multiple dynamic bonding interactions, the composite elastomers demonstrated strong mechanical performance (with a strength of 31.45 MPa and elongation of 1167.73%) and ultrafast photothermal toughness self-healing performance (20 s and an efficiency of 94.34%). The introduction of MoO3-x nanowires allows the construction of unique three-dimensional cross-linked nanonetworks that can move and regulate interfacial dynamic interactions under 808 nm infrared laser stimulation, resulting in controlled mechanical and healing performance. Therefore, such special elastomers with strong photothermal responses and mechanical properties are expected to be useful in next-generation biological antibacterial materials, wearable devices, and artificial muscles.

Encoding spatiotemporal asymmetry in artificial cilia with a ctenophore-inspired soft-robotic platform.

A remarkable variety of organisms use metachronal coordination (i.e. numerous neighboring appendages beating sequentially with a fixed phase lag) to swim or pump fluid. This coordination strategy is used by microorganisms to break symmetry at small scales where viscous effects dominate and flow is time-reversible. Some larger organisms use this swimming strategy at intermediate scales, where viscosity and inertia both play important roles. However, the role of individual propulsor kinematics-especially across hydrodynamic scales-is not well-understood, though the details of propulsor motion can be crucial for the efficient generation of flow. To investigate this behavior, we developed a new soft robotic platform using magnetoactive silicone elastomers to mimic the metachronally coordinated propulsors found in swimming organisms. Furthermore, we present a method to passively encode spatially asymmetric beating patterns in our artificial propulsors. We investigated the kinematics and hydrodynamics of three propulsor types, with varying degrees of asymmetry, using Particle Image Velocimetry and high-speed videography. We find that asymmetric beating patterns can move considerably more fluid relative to symmetric beating at the same frequency and phase lag, and that asymmetry can be passively encoded into propulsors via the interplay between elastic and magnetic torques. Our results demonstrate that nuanced differences in propulsor kinematics can substantially impact fluid pumping performance. Our soft robotic platform also provides an avenue to explore metachronal coordination at the meso-scale, which in turn can inform the design of future bioinspired pumping devices and swimming robots.

Next-Generation Structural Adhesives Composed of Epoxy Resins and Hydrogen-Bonded Styrenic Block Polymer-Based Thermoplastic Elastomers.

Structural adhesives are currently applied in the assembly of automobiles, aircraft, and buildings. In particular, epoxy adhesives are widely used due to their excellent mechanical strength and durability. However, cured epoxy resins are typically rigid and inflexible; thus, they have low peel and impact strength. In this study, tough cured epoxy adhesives were developed by mixing a liquid epoxy prepolymer (EP) and polystyrene-b-polyisoprene-b-polystyrene (SIS). SIS is a block polymer-based thermoplastic elastomer (TPE) composed of polystyrene (S) soluble in liquid EP and polyisoprene (I) insoluble in liquid EP, where S and I have a glass transition temperature that is higher and lower than room temperature, respectively. In addition, cured adhesives tougher than the cured adhesives containing SIS were prepared by mixing liquid EP and SIS with hydrogen-bonding groups in the I block (h-SIS). Transmission electron microscopy (TEM) observations revealed mixed S/cured EP domains, with a d-spacing of several tens of nanometers, and cured EP domains, with diameters of one hundred to several hundred nanometers, that were macroscopically dispersed in the I or hydrogen-bonded I matrix of the cured adhesive containing SIS or h-SIS. The lap shear, peel, and impact strength of cured neat EP (EP*) were 23 MPa, 45 N/25 mm, and 0.62 kN/m, respectively. Meanwhile, the cured adhesive containing 16.5 wt % SIS exhibited the slightly lower lap shear strength of 17 MPa compared to that of cured EP*, whereas the peel and impact strength of the cured adhesive with SIS were 61 N/25 mm and 7.1 kN/m, respectively, both higher than those of EP*. Furthermore, the lap shear strength of the cured adhesive containing 15.5 wt % h-SIS was 21 MPa, which was similar to that of cured EP*. The cured adhesive with h-SIS also exhibited an excellent peel strength of 97 N/25 mm and an impact strength of 14 kN/m which was 22 times higher than that of cured EP*. Therefore, mixing liquid EP and SIS improved the cured adhesive properties and flexibility of the cured epoxy adhesives compared to the cured adhesive composed of neat EP, and further enhancement of the adhesive properties was achieved by mixing liquid EP and h-SIS with hydrogen-bonding groups instead of mixing with SIS.

Tracking the evolution of the morphology and stress distribution of SIS thermoplastic elastomers under tension using atomic force microscopy.

Styrene-based ABA-type triblock copolymers and their blends are widely investigated thermoplastic elastomers (TPEs). The design of tough TPE materials with high strength and resilience requires further clarification of the relationship between microstructure and macroscopic properties of stretched samples. Here, we applied atomic force microscopy (AFM)-based quantitative nanomechanical mapping to study the deformation behavior of poly(styrene-b-isoprene-b-styrene) blends under tension. The results indicated that the glassy polystyrene (PS) domains deformed and inhomogeneous stress distributions developed in the initial stretching stage. At 200% strain, the glassy PS domains started to crack. The change in the peak value in the JKR Young's modulus diagram during stretching was consistent with the stress - strain curve. Analysis of the particles before and after stretching suggested that the glassy domains separated and reorganized during stretching.

A tough thermoplastic elastomer (TPE) with high strength and resilience was developed using styrene-based triblock copolymers and their blends, with its high-performance mechanism analyzed through AFM-based quantitative nanomechanical mapping.

Stretchable Distributed Bragg Reflectors as Strain-Responsive Mechanochromic Sensors.

Mechanochromic materials exhibit color changes upon external mechanical stimuli, finding wide-ranging applications in colorimetric sensing, display technology, and anticounterfeiting measures. Many of these materials rely on fluorescence properties and therefore necessitate external optical or electrical excitation. However, for broader applicability, the detection of color changes by the naked eye only or without complicated detection instrumentation is highly desirable. Photonic crystals offer a promising avenue for attaining such performances. In this work, we present elastomeric distributed Bragg reflectors (DBRs) characterized by a series of photonic bandgaps exhibiting mechanochromic response from the near-infrared to the visible wavelengths. To achieve this, we engineered alternating thin films of a thermoplastic fluoropolymer and a styrene-butadiene copolymer using different elastomeric substrates to attain different behaviors. The reported system demonstrates a reversible and instantaneous shift of the photonic bandgaps in response to 100% strain in multiple deformation cycles. Comparing the DBR stress-strain response with the optical strain response confirms a mechanochromic sensitivity of ∼1.7-6.9 nm/% and ∼80 nm/MPa, with an optical Poisson's ratio in the range 0.3-0.7. All these properties are spectrally dependent, as demonstrated by exploiting the properties of different diffraction order photonic band gaps.

Modulating alginate-polyurethane elastomer properties: Influence of NCO/OH ratio with aliphatic diisocyanate.

This research addresses the need for enhanced biomaterials by investigating the influence of the NCO/OH ratio on sodium alginate-based polyurethane elastomers(Al-PUEs), offering novel insights into their structural, thermal, mechanical and swelling behavior. Al-PUEs were prepared by blending the chain extenders with key ingredients in a specific molar ratio using aliphatic HMDI and HTPB monomers. The chemical linkages, crystalline behavior, homogeneity, and surface morphology of PUEs were evaluated by FT-IR, XRD, SEM, and EDX analysis. Thermo-mechanical studies were performed using TGA, DSC and tensile testing. Swelling behavior and absorption analysis were analyzed in DMSO and water. The analysis indicated that the hydrophilicity and swelling behavior of the prepared PUEs were affected by the addition of sodium alginate content. The results exhibit the tailor-made network structure of Al-PUEs, resulting in better thermal stability, elasticity of materials via stress-strain behavior and marvelous characteristic features than traditional high-tech yields. Furthermore, the resulting Al-PUEs are potential candidates for biomedical implants.

Mechanochromic Displays Based on Photoswitchable Cholesteric Liquid Crystal Elastomers.

Stimuli responsive optical materials are attractive for many areas, from healthcare to art design. However, creating intricate color-changing patterns for visual information is still a challenge. This work describes the preparation of mechanochromic structural colored intricate pictures imprinted in cholesteric liquid crystal elastomers by using a chiral isosorbide molecular photo-switch. The photo-switch contains a photoisomerizable cinnamate moiety and was incorporated in a main chain liquid crystal oligomer with photopolymerizable acrylate end groups. After coating, the structural colored film was irradiated with ultraviolet (UV) light in air causing E/Z isomerization of the cinnamate units leading to a redshift of the structural color of the film. A grayscale photomask was used to spatially control the photoisomerization reaction and imprint colorful pictures such as portraits and landscapes, in the cholesteric liquid crystal films with high resolution. Photopolymerization in a nitrogen atmosphere led to a mechanochromic cholesteric liquid crystal elastomer with striking structural colors that blueshift upon strain independently. The sharp details of the patterns were preserved even under deformation and the system returned to the initial state upon strain removal. Our work offers a simple photo-switch approach to prepare stimuli responsive optical polymers imprinted with color-changing pictures of unprecedented complexity.

Response Properties of Electrorheological Composite Hydrophilic Elastomers Based on Different Morphologies of Magnesium-Doped Strontium Titanate.

As smart materials, electrorheological elastomers (EREs) formed by pre-treating active electrorheological particles are attracting more and more attention. In this work, four Mg-doped strontium titanate (Mg-STO) particles with spherical, dendritic, flake-like, and pinecone-like morphologies were obtained via hydrothermal and low-temperature co-precipitation. XRD, SEM, Raman, and FT-IR were used to characterize these products. The results showed that Mg-STOs are about 1.5-2.0 µm in size, and their phase structures are dominated by cubic crystals. These Mg-STOs were dispersed in a hydrogel composite elastic medium. Then, Mg-STO/glycerol/gelatin electrorheological composite hydrophilic elastomers were obtained with or without an electric field. The electric field response properties of Mg-doped strontium titanate composite elastomers were investigated. We concluded that dendritic Mg-STO composite elastomers are high-performance EREs, and the maximum value of their energy storage was 8.70 MPa. The significant electrorheological performance of these products is helpful for their applications in vibration control, force transducers, smart structures, dampers, and other fields.

Microbial Biosynthesis of Medium-Chain-Length Polyhydroxyalkanoate (mcl-PHA) from Waste Cooking Oil.

Waste cooking oil is a common byproduct in the culinary industry, often posing disposal challenges. This study explores its conversion into the valuable bioplastic material, medium-chain-length polyhydroxyalkanoate (mcl-PHA), through microbial biosynthesis in controlled bioreactor conditions. Twenty-four bacterial isolates were obtained from oil-contaminated soil and waste materials in Mahd Ad-Dahab, Saudi Arabia. The best PHA-producing isolates were identified via 16S rDNA analysis as Neobacillus niacini and Metabacillus niabensis, with the sequences deposited in GenBank (accession numbers: PP346270 and PP346271). This study evaluated the effects of various carbon and nitrogen sources, as well as environmental factors, such as pH, temperature, and shaking speed, on the PHA production titer. Neobacillus niacini favored waste cooking oil and yeast extract, achieving a PHA production titer of 1.13 g/L, while Metabacillus niabensis preferred waste olive oil and urea, with a PHA production titer of 0.85 g/L. Both strains exhibited optimal growth at a neutral pH of 7, under optimal shaking -flask conditions. The bioreactor performance showed improved PHA production under controlled pH conditions, with a final titer of 9.75 g/L for Neobacillus niacini and 4.78 g/L for Metabacillus niabensis. Fourier transform infrared (FT-IR) spectroscopy and gas chromatography-mass spectrometry (GC-MS) confirmed the biosynthesized polymer as mcl-PHA. This research not only offers a sustainable method for transforming waste into valuable materials, but also provides insights into the optimal conditions for microbial PHA production, advancing environmental science and materials engineering.

Mesogen Organizations in Nematic Liquid Crystal Elastomers Under Different Deformation Conditions.

Liquid crystal elastomers (LCEs) exhibit unique mechanical properties of soft elasticity and reversible shape-changing behaviors, and so serve as potentially transformative materials for various protective and actuation applications. This study contributes to filling a critical knowledge gap in the field by investigating the microscale mesogen organization of nematic LCEs with diverse macroscopic deformation. A polarized Fourier transform infrared light spectroscopy (FTIR) tester is utilized to examine the mesogen organizations, including both the nematic director and mesogen order parameter. Three types of material deformation are analyzed: uniaxial tension, simple shear, and bi-axial tension, which are all commonly encountered in practical designs of LCEs. By integrating customized loading fixtures into the FTIR tester, mesogen organizations are examined across varying magnitudes of strain levels for each deformation mode. Their relationships with macroscopic stress responses are revealed and compared with predictions from existing theories. Furthermore, this study reveals unique features of mesogen organizations that have not been previously reported, such as simultaneous evolutions of the mesogen order parameter and nematic director in simple shear and bi-axial loading conditions. Overall, the findings presented in this study offer significant new insights for future rational designs, modeling, and applications of LCE materials.

High-performance electrically responsive artificial muscle materials for soft robot actuation.

Traditional robotic devices are often bulky and rigid, making it difficult for them to adapt to the soft and complex shapes of the human body. In stark contrast, soft robots, as a burgeoning class of robotic technology, showcase exceptional flexibility and adaptability, positioning them as compelling contenders for a diverse array of applications. High-performance electrically responsive artificial muscle materials (ERAMMs), as key driving components of soft robots, can achieve efficient motion and deformation, as well as more flexible and precise robot control, attracting widespread attention. This paper reviews the latest advancements in high-performance ERAMMs and their applications in the field of soft robot actuation, using ionic polymer-metal composites and dielectric elastomers as typical cases. Firstly, the definition, characteristics, and electro-driven working principles of high-performance ERAMMs are introduced. Then, the material design and synthesis, fabrication processes and optimization, as well as characterization and testing methods of the ERAMMs are summarized. Furthermore, various applications of two typical ERAMMs in the field of soft robot actuation are discussed in detail. Finally, the challenges and future directions in current research are analyzed and anticipated. This review paper aims to provide researchers with a reference for understanding the latest research progress in high-performance ERAMMs and to guide the development and application of soft robots. STATEMENT OF SIGNIFICANCE.

Highly Stretchable, Transparent, Self-Healing Ion-Conducting Elastomers for Long-Term Reliable Human Motion Detection.

The flexible electronic sensor is a critical component of wearable devices, generally requiring high stretchability, excellent transmittance, conductivity, self-healing capability, and strong adhesion. However, designing ion-conducting elastomers meeting all these requirements simultaneously remains a challenge. In this study, a novel approach is presented to fabricate highly stretchable, transparent, and self-healing ion-conducting elastomers, which are synthesized via photo-polymerization of two polymerizable deep eutectic solvents (PDESs) monomers, i.e., methacrylic acid (MAA)/choline chloride (ChCl) and itaconic acid (IA)/ChCl. The as-prepared ion-conducting elastomers possess outstanding properties, including high transparency, conductivity, and the capability to adhere to various substrates. The elastomers also demonstrate ultra-stretchability (up to 3900%) owing to a combination of covalent cross-linking and noncovalent cross-linking. In addition, the elastomers can recover up to 3250% strain and over 94.5% of their original conductivity after self-healing at room temperature for 5 min, indicating remarkable mechanical and conductive self-healing abilities. When utilized as strain sensors to monitor real-time motion of human fingers, wrist, elbow, and knee joints, the elastomers exhibit stable and strong repetitive electrical signals, demonstrating excellent sensing performance for large-scale movements of the human body. It is anticipated that these ion-conducting elastomers will find promising applications in flexible and wearable electronics.

Engineering of Reversibly Cross-Linked Elastomers Toward Flexible and Recyclable Elastomer/Carbon Fiber Composites with Extraordinary Tearing Resistance.

Carbon fiber (CF)-reinforced polymers (CFRPs) demonstrate potential for use in personal protective equipment. However, existing CFRPs are typically rigid, nonrecyclable, and lack of tearing resistance. In this study, flexible, recyclable, and tearing resistant polyurethane (PU)-CF composites are fabricated through complexation of reversibly cross-linked PU elastomer binders with CF fabrics. The PU-CF composites possess a high strength of 767 MPa and a record-high fracture energy of 2012 kJ m-2. The high performance of the PU-CF composites originates from the well-engineered PU elastomer binders that are obtained by cross-linking polytetrahydrofuran chains with in situ-formed nanodomains composed of hierarchical supramolecular interactions of hydrogen and coordination bonds. When subjected to tearing, the force concentrated on the damaged regions of the PU-CF composites can be effectively distributed to a wider area through the PU binders, leading to a significantly enhanced tearing resistance of the composites. The strong interfacial adhesion between PU binders and the CF fabrics enables the fracture of the CF in bundles, thereby significantly enhancing the strength and fracture energy of the composites. Because of the dynamic nature of the PU elastomer binders, the PU-CF composites can be recycled through the dissociation of the PU elastomer binders.

Application of Silicone in Ophthalmology: A Review.

This paper reviews the latest trends and applications of silicone in ophthalmology, especially related to intraocular lenses (IOLs). Silicone, or siloxane elastomer, as a synthetic polymer, has excellent biocompatibility, high chemical inertness, and hydrophobicity, enabling wide biomedical applications. The physicochemical properties of silicone are reviewed. A review of methods for mechanical and in vivo characterization of IOLs is presented as a prospective research area, since there are only a few available technologies, even though these properties are vital to ensure medical safety and suitability for clinical use, especially if long-term function is considered. IOLs represent permanent implants to replace the natural lens or for correcting vision, with the first commercial foldable lens made of silicone. Biological aspects of posterior capsular opacification have been reviewed, including the effects of the implanted silicone IOL. However, certain issues with silicone IOLs are still challenging and some conditions can prevent its application in all patients. The latest trends in nanotechnology solutions have been reviewed. Surface modifications of silicone IOLs are an efficient approach to further improve biocompatibility or to enable drug-eluting function. Different surface modifications, including coatings, can provide long-term treatments for various medical conditions or medical diagnoses through the incorporation of sensory functions. It is essential that IOL optical characteristics remain unchanged in case of drug incorporation and the application of nanoparticles can enable it. However, clinical trials related to these advanced technologies are still missing, thus preventing their clinical applications at this moment.

Coiled Carbon Nanotube Fibers Sheathed by a Reinforced Liquid Crystal Elastomer for Strong and Programmable Artificial Muscles.

Fibers of liquid crystal elastomers (LCEs) as promising artificial muscle show ultralarge and reversible contractile strokes. However, the contractile force is limited by the poor mechanical properties of the LCE fibers. Herein, we report high-strength LCE fibers by introducing a secondary network into the single-network LCE. The double-network LCE (DNLCE) shows considerable improvements in tensile strength (313.9%) and maximum actuation stress (342.8%) compared to pristine LCE. To facilitate the controllability and application, a coiled artificial muscle fiber consisting of DNLCE-coated carbon nanotube (CNT) fiber is prepared. When electrothermally driven, the artificial muscle fiber outputs a high actuation performance and programmable actuation. Furthermore, by knitting the artificial muscle fibers into origami structures, an intelligent gripper and crawling inchworm robot have been demonstrated. These demonstrations provide promising application scenarios for advanced intelligent systems in the future.

Tough and Elastic Cellulose Composite Hydrogels/Films for Flexible Wearable Sensors.

Cellulose and its composites, despite being abundant and sustainable, are typically brittle with very low flexibility/stretchability. This study reports a solution processing method to prepare porous, amorphous, and elastic cellulose hydrogels and films. Native cellulose dissolved in a water-ZnCl2 mixture can form ionic gels through in situ polymerization of acrylic acid (AA) to poly(acrylic acid) (PAA). The addition of up to 30 vol % AA does not change the solubility of cellulose in the water-ZnCl2 mixture. After polymerization, the formation of interpenetrated networks, resulting from the chemical cross-linking of PAA and the ionic/coordination binding among cellulose/PAA and ZnCl2, gives rise to strong, transparent, and ionically conductive hydrogels. These hydrogels can be used for wearable sensors to detect mechanical deformation under stretching, compression, and bending. Upon removal of ZnCl2 and drying the gels, semitransparent amorphous cellulose composite films can be obtained with a Young's modulus of up to 4 GPa. The rehydration of these films leads to the formation of tough, highly elastic composites. With a water content of 3-10.5%, cellulose-containing films as strong as paper also show typical characteristics of elastomers with an elongation of up to 1300%. Such composite films provide an alternative solution to resolving the material sustainability of natural polymers without compromising their mechanical properties.