Tough Hydrogels Research Articles

Tough double-network hydrogels with excellent frictional properties based on the in-suit inhibition strategy for biomedical applications

Osteoarthritis (OA) is one of the most common joint disorders all over the world and hydrogels could be an effective tool to solve this problem. In this work, we explore the mechanism of tribology properties of double-network hydrogel (DN hydrogel) under effect of free radical polymerization inhibitors. Fe3+ is added to the DN hydrogel as highly efficient and easily adjustable inhibitor, and the friction coefficient can be reduced to 0.0038 by adjusting the concentration. Even after 6 h of continuous tribological testing, the DN hydrogel remains a surprising sustained superlubricity. Furthermore, the strength of the hydrogel can reach 2.36 MPa, which is 20 times higher than that of the single-network hydrogel (SN hydrogel). The introduction of the inhibitor reduces covalent crosslinking that enables the hydrogel to form a sparser mesh structure conducive to the reduction of the friction coefficient, especially the additional physical cross-linking delivered from the electrostatic interaction between Fe3+ and carboxyl groups increases strength. The optimum concentration of Fe3+ is explored to achieve the synergetic improvement of lubricative and mechanical properties. This work opens innovative technology routes for developing superlubricious and tough hydrogels, which is a brighter future for artificial cartilage applications.

Strong and tough conductive hydrogels via an amphiphilic macromolecular crosslinker for flexible strain sensor

The strength and toughness of hydrogel are usually achieved through the synergy of chemical cross-linking and physical cross-linking from multi-component contributions. However, there are few reports on hydrogels that rely on a single component to obtain two cross-linked structures. Herein, we successfully synthesized an amphiphilic macromolecular crosslinker (polyoxyethylene 20 oleyl ether acrylate (O20AC)), and introduced it into a system composed of acrylamide (AAm), sodium chloride (NaCl) and water to prepare the P(AAm-O20AC)/NaCl hydrogel with high strength, outstanding toughness, and excellent good conductivity. Notably, the O20AC possess both crosslinker properties, which not only provide hydrogels with a stable chemical cross-linking network, but also its long hydrophobic chain act as physical crosslinking points to give the hydrogel a new pathway of energy dissipation.Depending on the O20AC crosslinker, the P(AAm-O20AC)/NaCl hydrogels exhibit good strength (tensile stress 714.46 kPa), toughness (elongation at break 3005 %), and fatigue resistance (overlap of hysteresis curves in repeated loading–unloading cycles). Besides, the existence of sodium ions and chloride ions also provides the hydrogel with highly sensitive deformation-dependent conductivity (GF is 5.8 in the 400 %-500 % strain range). Collectively, the strategy of preparing chemical and physical double-crosslinked hydrogels by amphiphilic O20AC will provide a bran-new insights for the development of hydrogel sensing materials.

Fabrication and characterization of sodium alginate-silicon nitride-PVA composite biomaterials with damping properties

Silicon nitride is utilized clinically as a bioceramic for spinal fusion cages, owing to its high strength, osteoconductivity, and antibacterial effects. Nevertheless, silicon nitride exhibits suboptimal damping properties, a critical factor in mitigating traumatic bone injuries and fractures. In fact, there is a scarcity of spinal implants that simultaneously demonstrate proficient damping performance and support osteogenesis. In our study, we fabricated a novel sodium alginate-silicon nitride/poly(vinyl alcohol) (SA-SiN/PVA) composite scaffold, enabling enhanced energy absorption and rapid elastic recovery under quasi-static and impact loading scenarios. Furthermore, the study demonstrated that the incorporation of physical and chemical cross-linking significantly improved stiffness and recoverable energy dissipation. Concerning the interaction between cells and materials, our findings suggest that the addition of silicon nitride stimulated osteogenic differentiation while inhibiting Staphylococcus aureus growth. Collectively, the amalgamation of ceramics and tough hydrogels facilitates the development of advanced composites for spinal implants, manifesting superior damping, osteogenic potential, and antibacterial properties. This approach holds broader implications for applications in bone tissue engineering.

Engineering Tough Supramolecular Hydrogels with Structured Micropillars for Tunable Wetting and Adhesion Properties.

Soft-lithography is widely used to fabricate microstructured surfaces on plastics and elastomers for designable physical properties such as wetting and adhesions. However, it remains a big challenge to construct high-aspect-ratio microstructures on the surface of hydrogels due to the difficulty in demolding from the gel with low strength and stiffness. Demonstrated here is the engineering of tough hydrogels by soft-lithography to form well-defined micropillars. The mechanical properties of poly(acrylamide-co-methacrylic acid) hydrogels with dense hydrogen-bond associations severely depend on temperature, with Young's modulus increasing from 8.1MPa at 15°C to 821.8MPa at -30°C, enabling easy demolding at low temperatures. Arrays of micropillars are maintained on the surface of the gel, and can be used at room temperature when the gel restores soft and stretchable. The hydrogel also exhibits good shape-memory property, favoring tailoring the morphology with a switchable tilt angle of micropillars. Consequently, the hydrogel shows tunable wetting and adhesion properties, as manifested by varying contact angles and adhesion strengths. These surface properties can also be tuned by geometry and arrangement of micropillars. This facile strategy by harnessing tunable viscoelasticity of supramolecular hydrogels should be applicable to other soft materials, and broaden their applications in biomedical and engineering fields.

Design principles for strong and tough hydrogels

Design principles for strong and tough hydrogels

Fermentation-inspired macroporous and tough gelatin/sodium alginate hydrogel for accelerated infected wound healing

Gelatin and sodium alginate (SA) are two important biological macromolecules, exhibiting excellent biocompatibility and gel-forming ability. However, traditional SA and gelatin hydrogel displays limited mass transport, low porosity, instability, and poor mechanical properties extremely restricted their therapeutic effect and application scenarios. Herein, microbial fermentation and synergistic toughening strategies were used for preparing macroporous and tough hydrogel. The study investigated the fermentation and toughening conditions of hydrogel. The hydrogel composed of CaCl2 cross-linked physically network and EDC/NHS cross-linked covalently network, exhibiting significantly improved mechanical properties, and excellent recovery efficiency. In addition, the hydrogel has a hierarchical macroporous structure of 100–500 μm, demonstrating high porosity of 10 times, swelling rate of 1541.0 %, and high mass infiltration capability. Further, after Ag+ treatment, the macroporous hydrogel dressing showed outstanding biocompatibility. Compared with non-porous hydrogel, the resulting macroporous hydrogel dressing displayed high antibacterial and antioxidant properties. It could effectively alleviate intracellular ROS formation induced by H2O2.In vivo experiments indicated that it has significantly better effect than non-porous hydrogel in accelerating wound healing. The overall results suggest that the gelatin/SA-based macroporous and tough hydrogel proposed in this study holds excellent prospects for application in wound dressings.

MXene Crosslinked Hydrogels with Low Hysteresis Conferred by Sliding Tangle Island Strategy.

Single-network hydrogels are often too fragile to withstand mechanical loading, whereas double-network hydrogels typically exhibit significant hysteresis during cyclic stretching-releasing process due to the presence of a sacrificial network. Consequently, it is a considerable challenge for designing hydrogels that are both low in hysteresis and high in toughness for applications requiring dynamic mechanical loads. Herein, the study introduced a novel "sliding tangle island" strategy for creating tough and low-hysteresis hydrogels, which are prepared through in situ polymerization of highly concentrated acrylamides (AM) to form numerous entanglements within the MXene spacing without any chemical crosslinker. The MXene entangled with long polyacrylamide (PAM) chains to form tangle island that served as a relay station to transmit stress to neighboring molecular chains. This mechanism helps alleviate stress concentration and enhances energy dissipation efficiency, thereby reducing mechanical hysteresis. The resulting hydrogel exhibited exceptional properties, including high stretchability (≈900%), low hysteresis (less than 7%), high toughness (1.34MJm-3), and excellent sensing performance to rival the commercial hydrogel electrode. Therefore, this work sheds light on feasible design of energy dissipation structure to reduce the hysteresis of the composite hydrogels.

An environment-stable and tough wearable sensor enabled by xanthan gum-assisted hydrogel

Wearable sensors based on ionic hydrogels have attracted increasing attention, but practical application is often hampered by poor environmental tolerance. Here, an environment-stable and tough hydrogel was constructed by introducing glycerin, sodium chloride and xanthan gum into a polyvinyl alcohol hydrogel network. Hydrogen bonds were formed among glycerin, xanthan gum and polyvinyl alcohol chains to enhance the toughness of hydrogel. Furthermore, the salting-out effect of polyvinyl alcohol chains induced by sodium chloride also improved the strength of hydrogel. Besides, the hydrogel was highly sensitive to mechanical deformation of tensile and compressive strain. The obtained hydrogel with sensitivity was capable of serving as a wearable sensor for monitoring human motions including speaking, bending articulation and so on. Notably, the hydrogel still maintained flexibility, toughness and conductivity under subzero or ambient conditions for a long time. This simple method paves an effective way for designing environment-stable and tough hydrogels.

Rapid Preparation Triggered by Visible Light for Tough Hydrogel Sensors with Low Hysteresis and High Elasticity: Mechanism, Use and Recycle-by-Design.

Hydrogels have emerged as promising candidates for flexible devices and water resource management. However, further applications of conventional hydrogels are restricted due to their limited performance and lack of a recycling strategy. Herein, a tough, flexible, and recyclable hydrogel sensor via a visible-light-triggered polymerization is rapidly created. The Zn2+ crosslinked terpolymer is in situ polymerized using g-C3N4 as the sole initiator to form in situ chain entanglements, endowing the hydrogels with low hysteresis and high elasticity. In the use phase, the hydrogel sensor exhibited high ion conductivity, excellent mechanical properties, fast responsiveness, high sensitivity, and remarkable anti-fatigue ability, making it exceptionally effective in accurately monitoring complex human movements. At the end-of-life (EOL), leveraging the synergy between the photodegradation capacity of g-C3N4 and the adsorption function of the hydrogel matrix, the post-consumer hydrogel is converted into water remediation materials, which not only promoted the rapid degradation of organic pollutants, but also facilitated collection and reuse. This innovative strategy combined in situ entangling reinforcement and tailored recycle-by-design that employed g-C3N4 as key blocks in the hydrogel to achieve high performance in the use phase and close the loop through the reutilization at EOL, highlighting the cost-effective synthesis, specialized structure, and life cycle management.

Sustainable highly stretchable and tough gelatin-alkali lignin hydrogels for scaffolding and 3D printing applications

Hydrogels and bioinks obtained from gelatin (Gel) generally present poor mechanical properties and require a series of time-consuming and stepwise chemical processes to exhibit improved elasticity and resistance to fatigue. Alkali lignin (AL) is an underutilized by-product of the paper and pulp industry. It is a widely available and inexpensive biomaterial that presents enormous potential for high-value applications owing to its ease of chemical modification and unique naturally occurring polyaromatic structure. This work aims to develop different GelAL hydrogel formulations with a single-step method that are innovative and sustainable. The results obtained from the mechanical, rheological, and degradation studies of the developed GelAL hydrogels demonstrated that their properties can be easily modified and tuned using straightforward processing techniques, allowing these stretchable and tough hydrogels to be used as bioinks in 3D printing. The modulation of mechanical properties through hydrogel formulations is a result of interactions between the Gel and AL which can be associated with the interplay of anionic sulfonates in AL and the arginine and lysine residues from Gel. The tensile stress at the break for the Gel20AL10 formulation was 32% higher than the value for Gel20AL5 and 157% higher than that of Gel10AL10. The elongation at break also decreased as it averaged 659 ± 149% for the Gel20AL10 formulation, which is 20% more than that of Gel20AL5 and 55% more than the average elongation at break of Gel10AL10. Further zeta potential measurements and quartz crystal microbalance with energy dissipation studies demonstrated that Gel and AL seem to form neutral complexes when mixed. These assays support the idea that AL and Gel are readily bound through weak interactions, and chemical crosslinking strategies need to be considered when degradability and mechanical properties tuning are envisioned. Altogether, these high-performance GelAL hydrogels display mechanical properties similar to soft tissues with high elasticity beyond that of natural hydrogels and fulfill the requirements of a broad range of biomedical and tissue engineering scaffolding applications.

Mussel-Inspired Self-Adhesive and Tough Hydrogels for Effectively Cooling Solar Cells and Thermoelectric Generators.

Adhesive hydrogel-based evaporative cooling, which necessitates no electricity input, holds promise for reducing energy consumption in thermal management. Herein, inspired by the surface attachment of mussel adhesive proteins via abundant dynamic covalent bonds and noncovalent interactions, we propose a facile strategy to fabricate a self-adhesive cooling hydrogel (Li-AA-TA-PAM) using a copolymer of acrylamide (AM) and acrylic acid (AA) as the primary framework. The monomers formed hydrogen bonds between their carboxyl and amide groups, while tannic acid (TA), rich in catechol groups, enhances the adhesion of the hydrogel through hydrogen bonding. The hydrogel demonstrated strong adhesion to various material surfaces, including plastic, ceramic, glass, and metal. Even under high-speed rotation, it still maintains robust adhesion. The adhesion strength of the Li-AA-TA-PAM hydrogel to aluminum foil reached an impressive value of 296.875 kPa. Interestingly, the excellent contact caused by robust adhesion accelerates heat transfer, resulting in a rapid cooling performance, which mimics the perspiration of mammals. Lithium bromide (LiBr) with hydroactively sorptive sites is introduced to enhance sorption kinetics, thereby extending the effective cooling period. Consequently, the operation temperature of commercial polycrystalline silicon solar cells was reduced by 16 °C under an illumination of 1 kW m-2, and the corresponding efficiency of energy conversion was increased by 1.14%, thereby enhancing the output properties and life span of solar cells. The strategy demonstrates the potential for refrigeration applications using viscous gels.

Molecular simulation-guided and physics-informed constitutive modeling of highly stretchable hydrogels with dynamic ionic bonds

Adaptive polymers are being designed with dynamic molecular bonds or chain interactions to respond with external stimuli with unparalleled mechanical properties and multifunctionality. An elegant example is to substantially enhance the stretchability and toughness of hydrogels through the use of ionic bond interactions. To assist the materials design and applications, a predictive theory is in high demand. However, existing multi-scale mechanics models often rely on empirical assumptions and relationships derived from polymer chemistry or physics to describe the evolution of microscale details under external stimuli, which are challenging to be validated experimentally. This study introduces a new methodology to develop constitutive theories for stretchable hydrogels based on insights garnered from molecular dynamics (MD) simulations. The continuum-level viscoelastic theory establishes the thermodynamics framework for stress-strain relationships, while MD simulations inform the evolution mechanisms of microscale bond interactions and network rearrangements, such as the bond distance and network relaxation time. These insights are then properly formulated based on polymer physics principles and fed into the continuum-level model. The resulting constitutive theory closely captures the stress responses at various loading conditions observed in experiments, as well as the microscale system volume and bond distance uncovered in MD simulations. Parametric studies are conducted to investigate the influences of various loading and material parameters on the mechanical properties of the materials, including loading rates, network crosslinking density, maximum strain, and bonding strength. Overall, the study establishes the connection between microscale network structure and mechanical responses of stretchable hydrogels with dynamic ionic bonds. It also offers practical guidance for optimizing material structures and loading conditions to enhance energy absorption and dissipation capabilities. The modeling approach can be extended to the study of other adaptive polymers with different dynamic bonds to create more precise and physically meaningful constitutive models.

Mechanically Tough and Conductive Hydrogels Based on Gelatin and Z-Gln-Gly Generated by Microbial Transglutaminase.

Gelatin-based hydrogels with excellent mechanical properties and conductivities are desirable, but their fabrication is challenging. In this work, an innovative approach for the preparation of gelatin-based conductive hydrogels is presented that improves the mechanical and conductive properties of hydrogels by integrating Z-Gln-Gly into gelatin polymers via enzymatic crosslinking. In these hydrogels (Gel-TG-ZQG), dynamic π-π stacking interactions are created by the introduction of carbobenzoxy groups, which can increase the elasticity and toughness of the hydrogel and improve the conductivity sensitivity by forming effective electronic pathways. Moreover, the mechanical properties and conductivity of the obtained hydrogel can be controlled by tuning the molar ratio of Z-Gln-Gly to the primary amino groups in gelatin. The hydrogel with the optimal mechanical properties (Gel-TG-ZQG (0.25)) exhibits a high storage modulus, compressive strength, tensile strength, and elongation at break of 7.8 MPa at 10 °C, 0.15 MPa at 80% strain, 0.343 MPa, and 218.30%, respectively. The obtained Gel-TG-ZQG (0.25) strain sensor exhibits a short response/recovery time (260.37 ms/130.02 ms) and high sensitivity (0.138 kPa-1) in small pressure ranges (0-2.3 kPa). The Gel-TG-ZQG (0.25) hydrogel-based sensors can detect full-range human activities, such as swallowing, fist clenching, knee bending and finger pressing, with high sensitivity and stability, yielding highly reproducible and repeatable sensor responses. Additionally, the Gel-TG-ZQG hydrogels are noncytotoxic. All the results demonstrate that the Gel-TG-ZQG hydrogel has potential as a biosensor for wearable devices and health-monitoring systems.

A Biomimetic "Salting Out-Alignment-Locking" Tactic to Design Strong and Tough Hydrogel.

Recently, hydrogel-based soft materials have demonstrated huge potential in soft robotics, flexible electronics as well as artificial skins. Although various methods are developed to prepare tough and strong hydrogels, it is still challenging to simultaneously enhance the strength and toughness of hydrogels, especially for protein-based hydrogels. Herein, a biomimetic "salting out-alignment-locking" tactic (SALT) is introduced for enhancing mechanical properties through the synergy of alignment and the salting out effect. As a typical example, tensile strength and modulus of initially brittle gelatin hydrogels increase 940 folds to 10.12±0.50MPa and 2830 folds to 34.26±3.94MPa, respectively, and the toughness increases up to 1785 folds to 14.28±3.13MJ m-3. The obtained strength and toughness hold records for the previously reported gelatin-based hydrogel and are close to the tendons. It is further elucidated that the salting out effect engenders hydrophobic domains, while prestretching facilitates chain alignment, both synergistically contributing to the outstanding mechanical properties. It is noteworthy that the SALT demonstrates remarkable versatility across different salt types and polymer systems, thus opening up new avenues for engineering strong, tough, and stiff hydrogels.

A tough bioadhesive hydrogel supports sutureless sealing of the dural membrane in porcine and ex vivo human tissue.

Complete sequestration of central nervous system tissue and cerebrospinal fluid by the dural membrane is fundamental to maintaining homeostasis and proper organ function, making reconstruction of this layer an essential step during neurosurgery. Primary closure of the dura by suture repair is the current standard, despite facing technical, microenvironmental, and anatomic challenges. Here, we apply a mechanically tough hydrogel paired with a bioadhesive for intraoperative sealing of the dural membrane in rodent, porcine, and human central nervous system tissue. Tensile testing demonstrated that this dural tough adhesive (DTA) exhibited greater toughness with higher maximum stress and stretch compared with commercial sealants in aqueous environments. To evaluate the performance of DTA in the range of intracranial pressure typical of healthy and disease states, ex vivo burst pressure testing was conducted until failure after DTA or commercial sealant application on ex vivo porcine dura with a punch biopsy injury. In contrast to commercial sealants, DTA remained adhered to the porcine dura through increasing pressure up to 300 millimeters of mercury and achieved a greater maximum burst pressure. Feasibility of DTA to repair cerebrospinal fluid leak in a simulated surgical context was evaluated in postmortem human dural tissue. DTA supported effective sutureless repair of the porcine thecal sac in vivo. Biocompatibility and adhesion of DTA was maintained for up to 4 weeks in rodents after implantation. The findings suggest the potential of DTA to augment or perhaps even supplant suture repair and warrant further exploration.

Stretch-Induced Conductivity Enhancement in Highly Conductive and Tough Hydrogels.

The resistance of gels and elastomers increases significantly with tensile strain, which reduces conductive stability and restricts their use in stable and reliable electronics. Here, highly conductive tough hydrogels composed of silver nanowires (AgNWs), liquid metal (LM), and poly(vinyl alcohol) (PVA) are fabricated. The stretch-induced orientations of AgNWs, deformable LM, and PVA nanocrystalline create conductive pathways, enhancing the mechanical properties of the hydrogels, including increased ultimate fracture stress (13-33MPa), strain (3000-5300%), and toughness (390.9-765.1MJ m-3). Notably, the electrical conductivity of the hydrogels is significantly improved from 4.05 × 10-3 to 24 S m-1 when stretched to 4200% strain, representing a 6000-fold enhancement. The incorporation of PVA nanocrystalline, deformable LM, and AgNWs effectively mitigates stress concentration at the crack tip, thereby conferring crack propagation insensitivity and fatigue resistance to the hydrogels. Moreover, the hydrogels are designed with a reversible crosslinking network, allowing for water-induced recycling.

Tough polyamidoxime-nanocellulose supramolecular composite hydrogels for effective uranium extraction from seawater

It is highly desirable to synthesize high-performance composite hydrogels in a simple and economical manner for uranium extraction from seawater. In this study, tough polyamidoxime-nanocellulose (PAO-CNF) composite hydrogels are fabricated via supramolecular complexation. The nanostructured PAO domains are dispersed in the supramolecularly cross-linked CNF network, guaranteeing superior mechanical strength and satisfied uranium uptake in seawater. A high tensile strength of 4.3 MPa is retained for the composite hydrogels after immersion in seawater for 30 days, which is beneficial for long-term survival in the ocean. The uranium uptake capacity reaches 6.6 mg-U/g in seawater after 35-day adsorption, a synergistic effect from nanostructured PAO domains and hydrophilic CNF network. The tough supramolecular composite hydrogels have great potentials for uranium extraction from seawater, enabling sustainable development of energy and environment.

Strong, tough, high-release, and antibacterial nanocellulose hydrogel for refrigerated chicken preservation

Enormous amounts of food resources are annually wasted because of microbial contamination, highlighting the critical role of effective food packaging in preventing such losses. However, traditional food packaging faces several limitations, such as low mechanical strength, poor fatigue resistance, and low water retention. In this study, we aimed to prepare nanocellulose hydrogels with enhanced stretchability, fatigue resistance, high water retention, and antibacterial properties using soy hull nanocellulose (SHNC), polyvinyl alcohol (PVA), sodium alginate (SA), and tannic acid (TA) as raw materials. These hydrogels were applied in food packaging to extend the shelf life of refrigerated chicken. The structure and properties (e.g., mechanical, antibacterial, and barrier properties) of these hydrogels were characterized using different techniques. Fourier-transform infrared spectroscopy revealed the presence of hydrogen and ester bonds in the hydrogels, whereas scanning electron microscopy revealed the three-dimensional network structure of the hydrogels. Mechanical testing demonstrated that the SHNC/PVA/SA/TA-2 hydrogel exhibited excellent tensile properties (elongation = 160 %), viscoelasticity (storage modulus of 1000 Pa), and mechanical strength (compressive strength = 10 kPa; tensile strength = 0.35 MPa). Moreover, under weak acidic and alkaline conditions, the ester bonds of the hydrogel broke down with an increase in pH, improving its swelling and release properties. The SHNC/PVA/SA/TA-2 hydrogel displayed an equilibrium swelling ratio exceeding 300 %, with a release rate of >80 % for the bioactive substance TA. Notably, antibacterial testing showed that the SHNC/PVA/SA/TA-2 hydrogel effectively deactivated Staphylococcus aureus and Escherichia coli, prolonging the shelf life of refrigerated chicken to 10 d. Therefore, the SHNC/PVA/SA/TA hydrogels can be used in food packaging to extend the shelf life of refrigerated meat products. Their cost-effectiveness and simple preparation make them suitable for various applications in the food industry.

A tough and bioadhesive injectable hydrogel formed with maleimidyl alginate and pristine gelatin

Injectable hydrogels have wide applications in clinical practice. However, the development of tough and bioadhesive ones based on biopolymers, along with biofriendly and robust crosslinking strategies, still represents a great challenge. Herein, we report an injectable hydrogel composed of maleimidyl alginate and pristine gelatin, for which the precursor solutions could self-crosslink via mild Michael-type addition without any catalyst or external energy upon mixing. This hydrogel is tough and bioadhesive, which can maintain intactness as well as adherence to the defect of porcine skin under fierce bending and twisting, warm water bath, and boiling water shower. Besides, it is biocompatible, bioactive and biodegradable, which could support the growth and remodeling of cells by affording an extracellular matrix-like environment. As a proof of application, we demonstrate that this hydrogel could significantly accelerate diabetic skin wound healing, thereby holding great potential in healthcare.

Self-adhesive, ionic conductive, environmentally tolerant, and antibacterial phytic acid-reinforced zwitterionic hydrogels as flexible sensor applications

Ionic conductive hydrogels have attracted tremendous research interest for their intrinsic characteristics in the field of flexible sensors. However, the combination of multifunctionalities of high mechanical strength, satisfactory self-adhesiveness, ionic conductivity, anti-freezing, antibacterial properties, and biocompatibility remains a great challenge for the development of ionic conductive hydrogels. In this study, a novel ionic conductive hydrogel was developed by introducing highly conductive phytic acid (PA) to poly(sulfobetaine methacrylate) (polySBMA). PA molecules, as non-covalent crosslinkers and electrolytes in the polySBMA network, significantly improved the mechanical properties, self-adhesion, and electrical properties of the hydrogels. The optimal hydrogel displayed robust mechanical properties (tensile stress: 240.7 kPa), desirable adhesive strength (18.6 kPa to pig skin), and excellent ionic conductivity (2.44 S/m). Simultaneously, the presence of PA confers hydrogels with good antibacterial, anti-freezing properties and long-term environmental stability, and the hydrogels could remain soft even at -40 °C. Moreover, the hydrogel-based sensors showed high sensitivity (gauge factor up to 9.72), wide sensing range (≈400%), good stability, and accuracy for physical and physiological signals (tensile strain, pressure, fluid types and concentrations). This work has not only provided a simple strategy for fabricating tough and recoverable zwitterionic hydrogels, but also demonstrated the multifunctional properties of the zwitterionic hydrogels, which possess a great potential to fulfill flexible device applications.