Polymer Network Research Articles

A Strong and Tough Ion‐gel Enabled by Hierarchical Meshing and Ion Hybridizations Collaboration

AbstractIon‐gels, with inherent flexibility, tunable conductivity, and multi‐stimulus response, have attracted significant attention in flexible/wearable electronics. However, the design of ion‐gels that exhibit both strength and toughness is challenging. In this study, a novel ion‐gel design is proposed that mimics the hierarchical meshing structure of leaves in combination with ion hybridization. Polyacrylamide (PAM) is incorporated in TEMPO oxidized cellulose nanofibers (TOCNFs) clusters by in situ polymerization, generating a hydrogel with micro/nanoscale entangled networks. Replacement of water by a metal halide ionic liquid ([BMIm]ZnxCly) in the hydrogel resulted in the formation of an ion hybrid network with supramolecular interactions. The integration of the PAM/TOCNF polymer network with [BMIm]ZnxCly resulted in ion‐gels with high strength (5.9 MPa), toughness (22 MJ m−3), and enhanced elastic modulus (30 MPa) combined with non‐flammability, heat and cold resistance. While having fast responsiveness (36 ms) of sensing signal and stability of power supply even at 4000 cycle collisions. Stable signal output even at high (200 °C) /sub‐zero temperatures. The proposed strategy offers a new approach to the material design of flexible/wearable electronics.

Activated Phenyl Ester Vitrimers

AbstractAromatic esters are amongst the oldest known chemical motifs that allow for thermal (re)processing of thermosetting polymers. Moreover, phenyl esters are generally known as activated esters that do not require a catalyst to undergo acyl transfer reactions. Even though dynamic aromatic esters find applications in commercialized thermoset formulations, all‐aromatic esters have found limited use so far in the design of covalent adaptable networks (CAN) as a result of their high glass transition temperature (Tg) and specific curing process. Here, a strategy to include partly aromatic esters as dynamic cross‐links inside low Tg (−40 °C) thermosetting formulations, using aliphatic esters derived from para‐hydroxybenzoic acid, which serves as a highly activated phenol or as a reactive “phenylogous anhydride” is reported. A small molecule study shows that the activated phenyl ester bonds can readily exchange with free phenol moieties at 200 °C under catalyst‐free conditions, while the addition of a catalyst allows for a faster exchange. Robust and hydrophobic polymer networks are conveniently prepared via rapid thiol‐ene UV‐curing of unsaturated phenol esters. The obtained networks show high thermal stability (350 °C), fast processability, good water resistance, and low creep up to 120 °C, thus showing good promise as a platform for CAN.

Construction of Slide‐Ring Polymers Based on Pillar[5]Arene/Alkyl Chain Host−Guest Interactions

AbstractSlide‐ring polymers exhibit distinctive mechanical properties, making them highly promising for applications in emerging fields such as energy storage devices and smart sensing. However, existing slide‐ring polymer systems primarily rely on hydrophilic‐hydrophobic interactions to achieve ring‐axle interlocking in aqueous phases. This reliance limits the construction of slide‐ring networks mainly to water‐soluble polymers, excluding a diverse range of lipophilic polymers. Therefore, it is crucial to introduce efficient construction strategies that facilitate interpenetration in organic solvents, enabling the development of diverse slide‐ring polymers and expanding their range and applications. Herein, by utilizing the pillar[5]arene/alkyl chain host−guest interactions, we successfully facilitated the interpenetration of a pillar[5]arene and poly(caprolactone), enabling the efficient construction of two slide‐ring polymer networks in organic solvents. One of these two slide‐ring polymers demonstrates a unique network deformation mechanism along with outstanding mechanical properties compared with the control covalently cross‐linked polymer network, including maximum stress (4.43 vs 1.98 MPa), maximum strain (1285 vs 330 %), and toughness (35.4 vs 3.92 MJ/m3). More importantly, this strategy of making slide‐ring polymers is highly versatile, given the wide range of macrocyclic arenes and alkyl chain‐containing polymers it can accommodate.

Construction of Slide-Ring Polymers Based on Pillar[5]Arene/Alkyl Chain Host-Guest Interactions.

Slide-ring polymers exhibit distinctive mechanical properties, making them highly promising for applications in emerging fields such as energy storage devices and smart sensing. However, existing slide-ring polymer systems primarily rely on hydrophilic-hydrophobic interactions to achieve ring-axle interlocking in aqueous phases. This reliance limits the construction of slide-ring networks mainly to water-soluble polymers, excluding a diverse range of lipophilic polymers. Therefore, it is crucial to introduce efficient construction strategies that facilitate interpenetration in organic solvents, enabling the development of diverse slide-ring polymers and expanding their range and applications. Herein, by utilizing the pillar[5]arene/alkyl chain host-guest interactions, we successfully facilitated the interpenetration of a pillar[5]arene and poly(caprolactone), enabling the efficient construction of two slide-ring polymer networks in organic solvents. One of these two slide-ring polymers demonstrates a unique network deformation mechanism along with outstanding mechanical properties compared with the control covalently cross-linked polymer network, including maximum stress (4.43 vs 1.98 MPa), maximum strain (1285 vs 330 %), and toughness (35.4 vs 3.92 MJ/m3). More importantly, this strategy of making slide-ring polymers is highly versatile, given the wide range of macrocyclic arenes and alkyl chain-containing polymers it can accommodate.

Antimicrobial Peptide SAAP‐148‐Functionalized Hydrogels from Photocrosslinkable Polymers with Broad Antibacterial Activity

AbstractAntimicrobial peptides (AMPs) are promising alternatives to traditional antibiotics for treating skin wound infections. Nonetheless, their short half‐life in biological environments restricts clinical applicability. Covalent immobilization of AMPs onto suitable substrates offers a comprehensive solution, creating contact‐killing surfaces with long‐term functionality. Here, a copolymer of poly[(hydroxy ethyl acrylamide)‐co‐(4‐benzophenone acrylamide)‐co‐(pentafluorophenyl acrylate)‐co‐(ECOSURF EH‐3 acrylate)], in short poly(HEAAm‐co‐BPAAm‐co‐PFPA‐co‐EH3A), is synthesized by free radical polymerization. Subsequent modification of active ester groups with the amine groups of SAAP‐148, results in a copolymer, that is non‐cytotoxic to human lung fibroblasts. UV photocrosslinking of the benzophenone units yields a polymer network that forms a hydrogel after swelling with aqueous medium. Both the SAAP‐148‐modified polymer in solution and the photocrosslinked hydrogels show good antimicrobial activity against strains of Escherichia coli, Staphylococcus aureus, Pseudomonas aeruginosa, and Acinetobacter baumannii, including multidrug‐resistant strains, frequently found in wound infections. The covalent attachment of SAAP‐148 prevents leaching, ensuring sustained antimicrobial activity for at least 48 h in diluted human blood plasma and 14 days in PBS. This prolonged retention of antimicrobial activity in human blood plasma significantly enhances its clinical potential. Overall, this study shows the potential of the AMP‐functionalized photocrosslinkable polymer as antimicrobial wound dressings, providing an effective alternative to antibiotics.

A single-particle energy-conserving dissipative particle dynamics approach for simulating thermophoresis of nanoparticles in polymer networks.

The transport of nanoparticles in polymer networks has critical implications in biology and medicine, especially through thermophoresis in response to temperature gradients. This study presents a single-particle energy-conserving dissipative particle dynamics (seDPD) method by integrating a single-particle model into the energy-conserving DPD model to simulate the mesoscopic thermophoretic behavior of nanoparticles in polymer matrices. We first validate the newly developed seDPD model through comparisons with analytical solutions for nanoparticle viscosity, thermal diffusivity, and hydrodynamic drag and then demonstrate the effectiveness of the seDPD model in capturing thermophoretic forces induced by temperature gradients. The results show that nanoparticles driven by the Soret forces exhibit unique transport characteristics, such as drift velocity and diffusivity, leading to a significant acceleration of nanoparticle diffusion in the polymer network, which has been known as the giant acceleration of diffusion. Quantifying how nanoparticles move in flexible polymer networks sheds light on the interaction dynamics of nanoparticles within polymer networks, providing insight into nanoparticle behavior in complex environments that could be leveraged in various applications from drug delivery to material design.

Interplay between Hydrogen Bond Network and Entangled Network in Polymers During Stretching Based on Molecular Simulations

Interplay between Hydrogen Bond Network and Entangled Network in Polymers During Stretching Based on Molecular Simulations

Stereochemical Shape Morphing in Diels-Alder Polymer Networks.

The intrinsic reversibility of dynamic covalent bonding, such as the furan-maleimide Diels-Alder (DA) cycloaddition reactions, enables reprocessable, self-healing polymer materials that can be reconfigured via the mechanism of solid-state plasticity. In this work, the temperature-dependent exchange rates of stereochemically distinct endo and exo DA bonds are leveraged to achieve tunable, temperature- and stress-activated shape morphing in Diels-Alder polymer (DAP) networks. Through thermal annealing, ≈35% of endo DA isomers are converted in neat DAP networks to the thermodynamically favored exo form, achieving ≈97% exo after complete annealing at 60°C. This conversion results in a ≈1.7 fold increase in elastic modulus, from 1.7 to 3.0MPa, and significantly alters the stress relaxation and shape recovery behavior. Spatially resolved annealing, is further showcased enabling the precise control of spatial distributions of endo and exo DA bonds across planar geometries. The locally distinct concentrations of endo/exo isomers, achieved by temperature-induced conversion of endo DA isomers to the thermodynamically stable exo DA isomers, gave rise to the spatial distributions of stress relaxation rates and elastic strain recovery mismatch to enable controlled stereochemical shape morphing. This approach provides a simplified, thermally driven method for shape morphing, with potential applications in soft robotics and flexible electronics.

Vinylic-addition Polynorbornene-based Anion-Exchange Membranes with Semi-Interpenetrating Polymer Networks for Water Electrolysis

Vinylic-addition Polynorbornene-based Anion-Exchange Membranes with Semi-Interpenetrating Polymer Networks for Water Electrolysis

Scalable, Fast Light‐Responsive, and Excellent Color‐Retention Fiber‐Based Photochromic Wearables for Sustainable Photo‐Patterning and Information Security Encryption

AbstractFiber‐based photochromic wearables have attracted growing attention in sustainable photo‐patterning information displays, information security encryption, and optical data recording/storage. Molybdenum trioxide (MoO3) is one of the key photochromic materials that possesses good photochromic performance, nevertheless, it faces considerable challenges in preparing photochromic textiles with stable, scalable, and long color‐retention properties. In this work, a new kind of fiber‐based photochromic wearables is designed and developed by combining cotton fabric with a MoO3‐based self‐adhesive polymer network and long chain silyl group. The prepared photochromic wearable has exhibited excellent fatigue resistance and favorable reversibility (> 40 cycles), rapid light response (reach color saturation with a UV dose of 60 kJ m−2), outstanding color retention capability (> 90 days), and desirable biocompatibility (cell viability > 100%). In addition, the prepared photochromic textiles could maintain a fast light response and excellent color retention even after experiencing repeated washing (20 cycles). Moreover, the photo‐patterning photochromic wearables are verified by resisting the deterioration of acid solution, alkali solution, and sweat (pH 2.0–9.0) as well as keeping clear patterns under sunlight irradiation. As a demonstration of the application, fiber‐based photochromic wearables are made and employed for the sustainable applications of rewritable photo‐patterning and information security encryption.

HRMAS NMR for Studying Solvent-Induced Mobility of Polymer Chains and Metallocene Migration Into Low-Density Polyethylene (LDPE).

HRMAS (high-resolution magic angle spinning) nuclear magnetic resonance (NMR) spectroscopy of low-density polyethylene (LDPE) affords 1H and 13C NMR spectra with superior resolution. For acquiring HRMAS NMR spectra, the polymer is first swollen with representative organic solvents. Then, the samples are measured with a conventional solid-state NMR spectrometer in the wideline mode or at the low spinning speed of 2 kHz. Anisotropic interactions like CSA (chemical shift anisotropy) and dipolar interactions are reduced due to the additional mobility of the polymer chains in the presence of the solvent within the polymer network. The combined effect of this mobility and MAS leads to signals with substantially reduced halfwidths as compared to classic MAS of the dry polymer. With HRMAS, all signals of the polymer become visible, and the spectra can be used for a quick and easy assessment of the polymer swelling behavior in diverse solvents. Being able to characterize polymers on the molecular level, and identifying the solvents that penetrate the polymer network best, enables the study of post-synthesis modifications of the polymers. It is demonstrated by paramagnetic HRMAS that the metallocene nickelocene (Cp2Ni) penetrates the LDPE network along with the solvent and is homogeneously dispersed in the polymer. SEM images prove that the structure of the polymer is not altered by the presence of a solvent and Cp2Ni. The impact of the paramagnetic Cp2Ni on the 1H signal halfwidth and T1 time of LDPE is studied. HRMAS allows a quick assessment of metal complexes regarding their ability to penetrate the LDPE network and therefore supports future studies of catalytic polymer degradation.

Silver Nanoparticle-Decorated Cellulose Nanocrystal Reinforced Ionic Polymer Hydrogel With High Conductivity and Environmental Tolerance for Multifunctional Sensing and Emergency Alarm System.

Conductive hydrogels hold great promise for flexible electronics. However, the simultaneous achievement of satisfactory mechanical strength, outstanding environmental tolerance, high sensitivity, and multiple sensing applications in a single conductive hydrogel remains a significant challenge. Herein, ionic polymer-based hydrogels with a double conductive network consisting of [2-(methacryloyloxy)ethyl] trimethyl ammonium chloride (DMC), 2-hydroxyethyl acrylate (HEA) and silver nanoparticle decorated cellulose nanocrystal (CNC@Ag) are prepared by a facile one-pot method. The resultant hydrogel (CDH) exhibits high stretchability, satisfactory self-adhesion, excellent environment tolerance (from -60 to 60°C), long-term stability (60 days), effective UV-shielding, and strong antibacterial properties. Significantly, the CDH hydrogel displays high conductivity and rapid response due to its double conductive network of ionic polymer and CNC@Ag. Therefore, the CDH-assembled sensor can accurately detect signals from both strain and pressure deformations, exhibiting outstanding sensitivity and reliability for human motion detection, signal transmission, object recognition, and tactile sensing. More interestingly, collaborating with a development board, the CDH-based sensor can be developed as an emergency alarm to realize prompt alarms in dangerous situations. Overall, this work presents a strategy for the fabrication of conductive hydrogel with remarkable properties, making it possible for multifunctional sensing applications in wearable electronics.

Interpenetrating Polymer Network Hydrogels with Tunable Viscoelasticity and Proteolytic Cleavability to Direct Stem Cells In Vitro.

The dynamic nature of cellular microenvironments, regulated by the viscoelasticity and enzymatic cleavage of the extracellular matrix, remains challenging to emulate in engineered synthetic biomaterials. To address this, a novel platform of cell-instructive hydrogels is introduced, composed of two concurrently forming interpenetrating polymer networks (IPNs). These IPNs consist of the same basic building blocks - four-armed poly(ethylene glycol) and the sulfated glycosaminoglycan (sGAG) heparin - are cross-linked through either chemical or physical interactions, allowing for precise and selective tuning of the hydrogel's stiffness, viscoelasticity, and proteolytic cleavability. The studies of the individual and combined effects of these parameters on stem cell behavior revealed that human mesenchymal stem cells exhibited increased spreading and Yes-associated protein transcriptional activity in more viscoelastic and cleavable sGAG-IPN hydrogels. Furthermore, human induced pluripotent stem cell (iPSC) cysts displayed enhanced lumen formation, growth, and pluripotency maintenance when cultured in sGAG-IPN hydrogels with higher viscoelasticity. Inhibition studies emphasized the pivotal roles of actin dynamics and matrix metalloproteinase activity in iPSC cyst morphology, which varied with the viscoelastic properties of the hydrogels. Thus, the introduced sGAG-IPN hydrogel platform offers a powerful methodology for exogenous stem cell fate control.

Broadband Response Diaphragm Materials for Human Acoustics Engineering.

High-performance fiber-reinforced composite materials demonstrate great potential for manufacturing diaphragms in human-engineered acoustic loudspeakers. However, the notable scarcity of high-quality fibers and the uncontrollable nature of the diaphragm structure limit the production of high-quality sound that conforms to human hearing. In this study, a novel composite diaphragm material is devloped by integrating the swelling carboxymethyl cellulose microfiber (CMF) with the hot-melted sheath-core fiber (SCF) based on the "interpenetrating polymeric network" ("IPN") strategy. Simulation methods and Flory-Huggins theory are applied to explain the mechanism of fiber-structure-property interaction in composite diaphragm materials. Owing to the distinct microstructure, this bio-based diaphragm material shows superior mechanical characteristics, including low density (≈0.92gcm- 3), high tensile strength (≈235MPa), and high modulus (≈9.73GPa). Moreover, the loudspeaker mounted with bio-based diaphragm material exhibits enhanced sensitivity (≈82.6dB) and stable performance across a broad frequency spectrum. This study not only elucidates the multiphysics working principles of loudspeakers but also establishes a crucial connection between the physical properties of diaphragms and loudspeaker performance. It opens up new avenues for the design of high-performance bio-based loudspeaker diaphragms in high-fidelity (Hi-Fi) acoustic devices.

Molecular complex inspired design of an efficient copper(II)-containing robust porous polymers for electrochemical water oxidation

Homogeneous copper-bipyridine complexes have been reported as effective catalysts for water oxidation, demonstrating significant potential as alternatives to precious metal-based complexes. However, these complexes face long-term stability and product separation challenges similar to many homogeneous catalysts. Meanwhile, recent studies have underscored the potential of metalated polymer networks, which integrate the structural advantages of polymers with the functional benefits of metal species, making them highly attractive for various applications. Herein, we integrated copper-bipyridine units into porous polymer networks to overcome the limitations of copper-bipyridine complexes. We prepared a series of copper-incorporated polymers (TpBpy-Cux) for electrochemical water oxidation. The electrochemical properties of these polymers were tuned by varying the copper content, with TpBpy-Cu3 presenting the best performance among the samples studied. TpBpy-Cu3 demonstrated a low Tafel slope of 69 mV/decade, achieved a high Faradaic efficiency (FE) of 94 %, and exhibited exceptional stability over 1000 cyclic scans. This study offers insights into the design and optimization of metal-incorporated porous polymer networks building on the foundational understanding of their molecular counterparts for advanced catalytic applications.

Pillar[5]arene-based Polymer Network for Efficiently Removing Perfluorooctanoic Acid through Synergistic Binding Interactions.

Perfluorooctanoic acid (PFOA) is currently one of the most important chemicals posing environmental risks, and there is an urgent need to find methods to efficiently remove PFOA from environmental media. Here, two decaamino-pillar[5]arene-based fluorine-rich polymer networks, called FA2P-P and FA6P-P, were constructed using a convenient method. FA6P-P had an excellent ability to take up PFOA, and had a capacity of 1423 (mg PFOA) (g FA6P-P)-1, which is the second highest adsorption capacity reported for any PFOA sorbent. FA6P-P removed >99 % of the PFOA from a solution and decreased the PFOA concentration from 1000 μg L-1 in 5 min at an exceedingly low adsorbent loading of 0.7 mg L-1, giving a final PFOA concentration <4 ng L-1, which is lower than the most recent enforceable maximum concentration set by the United States Environmental Protection Agency. A high rate constant (kobs) of 55.8 g mg-1 h-1 was observed. Pillar[5]arene gives the material hydrophobic properties and also amino sites and hydrophobic chains, which are synergistic PFOA binding sites. The polymer was very stable and readily regenerated. The results indicated that pillar[5]arene-based porous organic polymer sorbents are excellent candidates for capturing PFOA.

In Situ Gel Polymer Electrolyte with Rapid Li+ Transport Channels and Anchored Anion Sites for High‐Current‐Density Lithium‐Ion Batteries

AbstractIn situ formed gel polymer electrolytes (GPEs) have advantages in safety and adaptability to current high‐voltage lithium‐ion batteries (LIBs). However, it is challenging for GPEs to achieve stable cycling at high current densities. A flexible framework is proposed for stable in situ GPE, by introducing ─CF3 groups to the polymer network to establish rapid Li+ transport channels, and incorporating secondary amine N─H groups to anchor anion. The obtained GPE exhibits a high ionic conductivity of 2.6 mS cm−1 and a high Li+ transference number of 0.67. The assembled Li||NCM811 cell demonstrates excellent rate performance, with a discharging capacity of 112.3 mAh g⁻¹ at 10C, and capacity retention of 87.6% after 260 cycles at 1C. Furthermore, the assembled graphite||NCM811 cell demonstrates excellent long‐term cycling stability with impressive capacity retention of 73.2% after 300 cycles 3C (1.8 mA cm−2). This work presents a promising approach to enhancing the cycling stability of GPEs for high‐voltage LIBs at high current density.

Fatigue Behavior of Polymer Nanocomposites under Low-Strain Cyclic Loading: Insights from Molecular Dynamics Simulation.

Understanding the structural evolution and bond-breaking behavior under cyclic loading is crucial for designing polymer nanocomposites (PNCs) with superior fatigue resistance. Coarse-grained models of PNCs filled with spherical carbon black nanoparticles (NPs) at varying filling fractions of φ were successfully constructed using molecular dynamics simulations. Structural and dynamic simulation results reveal that higher φ leads to increased aggregation of NPs and markedly restricts the relaxation behavior of the polymer matrix. Subsequently, fatigue testing of PNCs was conducted under low-strain cyclic tensile deformation, and the real-time bond-breaking behavior was tracked. The decay behavior of the bond number autocorrelation function was found to be accurately described by the KWW equation, enabling precise determination of the characteristic lifetime τf. With increasing φ, the dominant factor influencing bond-breaking behavior gradually shifts from the polymer network, including entanglements and cross-linking networks, to the filler network. This suggests the presence of a critical filling fraction φc where τf is maximized. For low-strain failure mechanisms, temperature field observations at varying cycles reveal that localized temperature rise emerges as the predominant factor. Furthermore, the mobility of both polymers and NPs increases with cycles. Specifically, the diffusion coefficient of polymer monomers shows a clear power-law relationship with the bond-breaking rate, characterized by . Finally, the stiffness of polymer chains significantly influences the fatigue behavior, evidenced by an initial increase followed by a decrease in the τf with increasing bending energy k. This behavior is attributed to the competitive relationship between high entanglement density at low k and enhanced preorientation at high k. In summary, this study provides a general paradigm for describing failure behavior under cyclic deformation and offers insights into fatigue mechanisms at the molecular level, thereby guiding the development of improved fatigue-resistant PNCs.

Environment-tolerant, inherently conductive and self-adhesive gelatin-based supramolecular eutectogel for flexible sensor

Although hydrogels have attracted increasing attention in the stretchable devices, the low adhesion properties and poor environmental adaptation still seriously restrict their development and application. Herein, we focused on the interaction between polymer networks with disperse media and their resultant influence on gel performance, and constructed self-adhesive and environment-tolerant gelatin/polyacrylamide supramolecular-polymer double-network (Gelatin/PAM SP-DN) eutectogels using multiple supramolecular interactions between natural macromolecule and well-designed deep eutectic solvent (DES). The dual networks of Gelatin/PAM SP-DN eutectogels produced significant supramolecular forces with DES, including hydrogen bonding and electrostatic interaction, contributing to enhance the energy dissipation capacity. Additionally, the Gelatin-PAM SP-DN eutectogels were more prone to generate strong bonding force to various substrates, showcasing both in-situ and ex-situ adhesion performance, and even being used for wet and underwater adhesion. The eutectogels revealed excellent environmental tolerance to maintain excellent mechanical flexibility, conductivity and adhesion at high and low temperatures, ensuring the constructed sensor to sensitively and reliably perceive strain, pressure and human motions over a wide temperature range. Also, the eutectogel demonstrated great potential as a temperature sensor. This work opens up a new horizon in the design of multifunctional and environment-tolerant natural macromolecule-based gel materials for flexible electronics, human-machine interaction and health diagnosis.

Human Muscle Inspired Anisotropic and Dynamic Metal Ion-Coordinated Mechanically Robust, Stretchable and Swelling-Resistant Hydrogels for Underwater Motion Sensing and Flexible Supercapacitor Application.

Mechanically robust and anisotropic conductive hydrogels have emerged as crucial components in the field of flexible electronic devices, since they possess high mechanical properties and intelligent sensing capabilities. However, the hydrogels often swell on exposure to aqueous medium because of their hydrophilicity, which compromises their mechanical properties. Additionally, the hydrogels' isotropic polymeric networks demonstrate isotropic ion transport, which significantly diminishes the sensing capabilities of electrical devices based on hydrogels. These factors greatly limit their use in flexible and wearable sensors. In this study, we have developed poly(acrylamide-co-maleic acid-co-butyl acrylate) based anisotropic hydrogels by prestretching and drying, followed by ionic cross-linking to fix the alignment. The anisotropic arrangement of the polymer network resulted in significant improvements in mechanical performance and electrical conductivity along the prestretching direction. This anisotropic hydrogel combines hydrophobic and metal ion-ligand interactions, enhancing the maximum tensile strength up to 11 MPa along the prestretching direction, about 3 times higher than in the perpendicular direction. The optimized 200% prestretched hydrogel exhibited high tensile strength (7 MPa), flexibility (fracture strain 370%), high toughness (16 MJ m-3) and antiswelling behavior in water (equilibrium swelling ratio 2% after 15 days). alongside higher conductivity (3 times higher) and strain sensing ability (4 times higher gauge factor) along the prestretching direction. The hydrogel demonstrated efficient and stable underwater sensing for underwater communication and to monitor human limb position and movement. The anisotropic hydrogel electrolyte-based flexible supercapacitor exhibited 117 Fg-1 specific capacitance at 0.5 Ag-1, and maximum energy density 5.85 Whkg-1, significantly higher than the corresponding values for the isotropic hydrogel-based device (88 F g-1 and 4.4 Whkg-1, respectively). This hydrogel mimics the structural design of unidirectionally oriented muscle fibers, showing better direction dependent functional properties than the corresponding isotropic hydrogel. The anti-swelling ability and retention of mechanical and conductive properties of these hydrogels in aqueous environment suggest long-term usage capability of these functional materials.