Zwitterionic Hydrogels Research Articles

Hybrid heart valves with VEGF-loaded zwitterionic hydrogel coating for improved anti-calcification and re-endothelialization.

With the aging of the population in worldwide, valvular heart disease has become one of the most prominent life-threatening diseases in human health, and heart valve replacement surgery is one of the therapeutic methods for valvular heart disease. Currently, commercial bioprosthetic heart valves (BHVs) for clinical application are prepared with xenograft heart valves or pericardium crosslinked by glutaraldehyde. Due to the residual cell toxicity from glutaraldehyde, heterologous antigens, and immune response, there are still some drawbacks related to the limited lifespan of bioprosthetic heart valves, such as thrombosis, calcification, degeneration, and defectiveness of re-endothelialization. Therefore, the problems of calcification, defectiveness of re-endothelialization, and poor biocompatibility from the use of bioprosthetic heart valve need to be solved. In this study, hydrogel hybrid heart valves with improved anti-calcification and re-endothelialization were prepared by taking decellularized porcine heart valves as scaffolds following grafting with double bonds. Then, the anti-biofouling zwitterionic monomers 2-methacryloyloxyethyl phosphorylcholine (MPC) and vascular endothelial growth factor (VEGF) were utilized to obtain a hydrogel-coated hybrid heart valve (PEGDA-MPC-DHVs@VEGF). The results showed that fewer platelets and thrombi were observed on the surface of the PEGDA-MPC-DHVs@VEGF. Additionally, the PEGDA-MPC-DHVs@VEGF exhibited excellent collagen stability, biocompatibility and re-endothelialization potential. Moreover, less calcification deposition and a lower immune response were observed in the PEGDA-MPC-DHVs@VEGF compared to the glutaraldehyde-crosslinked DHVs (Glu-DHVs) after subcutaneous implantation in rats for 30 days. These studies demonstrated that the strategy of zwitterionic hydrogels loaded with VEGF may be an effective approach to improving the biocompatibility, anti-calcification and re-endothelialization of bioprosthetic heart valves.

Highly Sensitive Zwitterionic Hydrogel Sensor for Motion and Pulse Detection with Water Retention, Adhesive, Antifreezing, and Self-Healing Properties.

The design and synthesis of conductive hydrogels with antifreezing, long-term stable, highly sensitive, self-healing, and reusable is a critical procedure to enable applications in flexible electronics, medical monitoring, soft robotics, etc. Herein, a novel zwitterionic composite hydrogel possessing antifreezing, fast self-healing performance, water retention, and adhesion was synthesized via a simple one-pot method. LiCl, as an electrolyte and antifreeze, was promoted to dissociate under the electrostatic interaction with zwitterions, resulting in the composite hydrogels with high electrical conductivity (7.95 S/m) and excellent antifreeze ability (-45.3 °C). Meanwhile, the composite hydrogels could maintain 97% of the initial water content after exposed to air (25 °C, 55% RH) for 1 week due to the presence of salt ions. Moreover, the active groups of zwitterions could form conformal adhesion between the composite hydrogels and skin, which was particularly crucial for the stable signal output of the sensor. The dynamic borate ester bonds, active group of zwitterions, and the hydrogen bond between different components could achieve rapid self-healing (2 h, self-healing efficiency to 97%) without any external intervention. Notably, the developed PBAS-Li (poly(vinyl alcohol) Borax/acrylamide/zwitterionic-LiCl) hydrogel not only succeeded in sensitively detecting human motions but also could precisely captured handwritings signals and subtle pulse waves on the neck and wrist. The above findings demonstrated the great potential of PBAS-Li hydrogels in the field of flexible electronic devices.

Zwitterionic liquid hydrogel sustained-release strategy for high-performance nanofiltration membrane

Controlling the diffusion of amine monomers plays a crucial role in fabricating well-defined architecture and high-performance nanofiltration (NF) membranes through interfacial polymerization (IP). Herein, a sustained-release strategy was proposed to regulate the interfacial polymerization through a zwitterionic liquid hydrogel transition layer. The hydrogel (Gel) was fabricated via in-situ one-step UV photo-initiated free-radical polymerization between 1-vinyl-3-ethylimidazolium chloride ([VEIm][Cl]) and 3-sulfopropyl methacrylate potassium salt (SMP) on the polyethersulfone (PES) substrate. The polyamide (PA) layer was then formed on the Gel layer by mitigating the diffusion of amine monomers. Low-field time-domain nuclear magnetic resonance (TD NMR) analysis demonstrated that the Gel layer significantly enhanced the water-absorbing capacity of the composite membrane. Positron annihilation lifetime spectroscopy (PALS) also confirmed the Gel-PA composite membrane possessed enlarged free volumes. The obtained Gel-PA composite membrane displayed a permeance of 13.22 L m−2 h−1 bar−1, a high Na2SO4 rejection of 98.23 %, a favorable NaCl/Na2SO4 selectivity of 49.75, outstanding long-term operational stability, and membrane antifouling properties. This sustained-release strategy provides a facile and feasible approach to controlling the IP process and obtaining high-performance nanofiltration membranes.

Recent Advances in Mechanical Reinforcement of Zwitterionic Hydrogels.

As a nonspecific protein adsorption material, a strong hydration layer provides zwitterionic hydrogels with excellent application potential while weakening the interaction between zwitterionic units, leading to poor mechanical properties. The unique anti-polyelectrolyte effect in ionic solution further restricts the application value due to the worsening mechanical strength. To overcome the limitations of zwitterionic hydrogels that can only be used in scenarios that do not require mechanical properties, several methods for strengthening mechanical properties based on enhancing intermolecular interaction forces and polymer network structure design have been extensively studied. Here, we review the works on preparing tough zwitterionic hydrogel. Based on the spatial and molecular structure design, tough zwitterionic hydrogels have been considered as an important candidate for advanced biomedical and soft ionotronic devices.

Microgel reinforced zwitterionic hydrogel coating for blood-contacting biomedical devices

Zwitterionic hydrogels exhibit eminent nonfouling and hemocompatibility. Several key challenges hinder their application as coating materials for blood-contacting biomedical devices, including weak mechanical strength and low adhesion to the substrate. Here, we report a poly(carboxybetaine) microgel reinforced poly(sulfobetaine) (pCBM/pSB) pure zwitterionic hydrogel with excellent mechanical robustness and anti-swelling properties. The pCBM/pSB hydrogel coating was bonded to the PVC substrate via the entanglement network between the pSB and PVC chain. Moreover, the pCBM/pSB hydrogel coating can maintain favorable stability even after 21 d PBS shearing, 0.5 h strong water flushing, 1000 underwater bends, and 100 sandpaper abrasions. Notably, the pCBM/pSB hydrogel coated PVC tubing can not only mitigate the foreign body response but also prevent thrombus formation ex vivo in rats and rabbits blood circulation without anticoagulants. This work provides new insights to guide the design of pure zwitterionic hydrogel coatings for biomedical devices.

A self-adhesive, self-healing zwitterionic hydrogel electrolyte for high-voltage zinc-ion hybrid supercapacitors

With the widespread application of portable electronic devices, high-performance supercapacitors have attracted enormous interest. Nevertheless, the previously reported supercapacitors typically suffer from a few disadvantages, such as the low energy density, irreversible breakage and poor interface combination between electrolyte and electrodes, restricting the development of high-performance supercapacitors. Herein, the betaine-based zwitterionic hydrogel electrolyte with excellent self-healing properties, anti-drying ability and mechanical flexibility was prepared for zinc-ion hybrid supercapacitor (ZIHS). Betaine enhanced the adhesion of zwitterionic hydrogel electrolytes, which promoted the interface bonding between electrolyte and electrode. Impressively, the ZIHS based on zwitterionic hydrogel electrolytes exhibited a wide electrochemical stability window of 2.2 V and a high energy density of 237.34 mAh/g. In addition, the ZIHS based on zwitterionic hydrogels possessed great self-healing ability, the self-healing efficiency achieved 88.3 % of the initial state after five cutting-healing cycles. This research will supply an effective strategy for the design of hydrogel-based supercapacitors with wide voltage windows, high energy density and reusability.

Anti-Swelling Zwitterionic Hydrogels as Multi-Modal Underwater Sensors and All-in-One Supercapacitors

Anti-Swelling Zwitterionic Hydrogels as Multi-Modal Underwater Sensors and All-in-One Supercapacitors

Kinetics‐Boosted Effect Enabled by Zwitterionic Hydrogel Electrolyte for Highly Reversible Zinc Anode in Zinc‐Ion Hybrid Micro‐Supercapacitors

AbstractDespite impressive merits of complementary charge‐storage mechanisms for aqueous Zn‐ion hybrid micro‐supercapacitors (ZHMSCs), it remains a challenge to solve dendrite and parasitic reactions issues of Zn anodes. Herein, a kinetics‐boosted strategy of Zn2+ transport and desolvation of hydrated Zn2+ is proposed by engineering zwitterionic P(AM‐co‐SBMA) hydrogel electrolyte (PASHE) for highly reversible Zn plating/stripping. Mechanically robust and chemically anchored PASHE features zwitterionic groups for constructing ion migration channels and immobilizing water molecules, which accelerates Zn2+ migration for an ultrahigh transfer number (0.84) and alleviates water‐related parasitic reactions. Theoretical calculations combined with experimental results reveal that sulfobetaine sulfonate anions endow PASHE with improved desolvation kinetics and the ability to coordinate Zn2+ flux and electric field distributions at the electrolyte–electrode interface. Thus, Zn anodes exhibit excellent electrochemical performance involving high average coulombic efficiency of 99.4% in Zn|PASHE|Cu cell as well as high cumulative capacity of 2000 mAh cm−2 (20 mA cm−2, 1 mAh cm−2) and depth of discharge of 80.9% (20 mA cm−2, 10 mAh cm−2) in Zn|PASHE|Zn cells. Furthermore, ZHMSCs based on PASHE deliver excellent flexibility and cyclability for energy‐storage applications. This work provides useful insights on hydrogel electrolyte engineering for developing high‐performance Zn anodes and derived energy‐storage devices.

A zwitterionic cellulose-based skin sensor for the real-time monitoring and antibacterial sensing wound dressing

Wound infection can induce inflammation and impede wound healing, being a major challenge in wound care management. A household device that can monitor infection in real time, prevent bacterial, and promote wound healing is highly desired but still rarely investigated. In this work, a novel zwitterionic cellulose-based hydrogel that enables continuously real-time monitoring and pro-healing of infected wound is designed. It is based on interpenetrating polymeric networks, including zwitterionic covalent bond network and physical bond network of carboxymethyl cellulose (CMC) with Ag+via metal-coordination interactions. When used as a sensing dressing, it is developed to exhibit pH-responsive and temperature-responsive properties for assessment of wound infection. Moreover, Ag+ can be released from carboxyl groups of CMC in response to the decrease of pH, killing bacteria and promoting wound healing. This zwitterionic carboxymethyl cellulose-based hydrogel sensor opens new avenues for domestic real-time monitoring and pro-healing of infected wound.

Non-ionic polar small molecules induced transition from elastic hydrogel via viscoelastic wormlike micelles to spherical micelles in zwitterionic surfactant systems

• A C18-tailed zwitterionic surfactant supramolecular hydrogel is constructed with OHSB and NaSal. • The non-ionic polar small molecules, TPA1, could control the microstructure and viscoelasticity of zwitterionic hydrogel. • Rheological measurement shows transition from Elastic Hydrogel via Viscoelastic Wormlike Micelles to Spherical micelles. • The microstructure of the system was analyzed by cryo-TEM and cryo-SEM. • The construction and transition mechanism were proposed, stating the detailed controlling process clearly. Supramolecular assembly determines the formation and transformation of soft materials. So far, the construction and transformation of conventional (<C20) zwitterionic surfactant elastic hydrogel have been a challenging and vital issue. In this work, a C18-tailed zwitterionic surfactant supramolecular hydrogel is constructed with N -octadecyl- N , N -dimethyl-3-ammonio-2-hydroxy-1-propane-sulfonate (OHSB) and sodium salicylate (NaSal). The N , N ,2,2-tetramethyl-1, 3-propanediamine (TPA1), as the non-ionic polar small molecules, were chosen to control the microstructure and macro-viscoelasticity of zwitterionic surfactant supramolecular hydrogel. With the addition of TPA1, the rheological properties and microstructural images of the OHSB/NaSal system show that the microstructure has changed from elastic hydrogels via viscoelastic wormlike micelles (WLMs) to spherical micelles. With the N , N , N’ , N’ -tetramethyl-1,3-propanediamine (TPA2), the isomer of TPA1, is added into OHSB/NaSal system in the same concentration, the difference in rheology and microstructure indirectly indicates the influence of hydrogen bonding on self-assembly. By systematically varying components, insight into the intermolecular interaction between OHSB, NaSal, and TPA1 and its effect on the microstructure during aggregation and transition are gained by the complementary use of 1 H NMR, rheological property, cryo-SEM, cryo-TEM, and DLS. We expect it to be a good model for conventional zwitterionic surfactant supramolecular hydrogel and a new method for controlling the internal nanostructure of micelles, which is helpful to understand the construction and finely tune of conventional zwitterionic surfactant supramolecular hydrogel and widen their applications.

Antifreezing Proton Zwitterionic Hydrogel Electrolyte via Ionic Hopping and Grotthuss Transport Mechanism toward Solid Supercapacitor Working at −50 °C

Hydrogel electrolyte is widely used in solid energy storage devices because of its high ionic conductivity, environmental friendliness, and non‐leakage property. However, hydrogel electrolyte is not resistant to freezing. Here, a high proton conductive zwitterionic hydrogel electrolyte with super conductivity of 1.51 mS cm–1 at −50 °C is fabricated by random copolymerization of acrylamide and zwitterionic monomer in the presence of 1 m H2SO4 and ethylene glycol (EG). The antifreezing performance and low temperature conductivity are ascribed to hydrogen bonds and ionic bonds between the components and water molecules in the system and can be tuned by changing the monomer ratio and EG contents. The proton hopping migration on the ionic group of the polymer chains and Grotthuss proton transport mechanism are responsible for the high proton conductivity while Grotthuss transport is dominated at the glassy state of the polymer chains. The electrolyte‐assembled supercapacitor (SC) offers high specific capacitance of 93.5 F g–1 at 25 °C and 62.0 F g–1 at −50 °C with a capacitance retention of 91.1% and 81.5% after 10 000 cycles, respectively. The SC can even work at −70 °C. The electrolyte outperforms most reported antifreezing hydrogel electrolytes and has high potential in low‐temperature devices.

Simple synthesis of soft, tough, and cytocompatible biohybrid composites

Collagen is the most abundant component of mammalian extracellular matrices. As such, the development of materials that mimic the biological and mechanical properties of collagenous tissues is an enduring goal of the biomaterials community. Despite the development of molded and 3D printed collagen hydrogel platforms, their use as biomaterials and tissue engineering scaffolds is hindered by either low stiffness and toughness or processing complexity. Here, we demonstrate the development of stiff and tough biohybrid composites by combining collagen with a zwitterionic hydrogel through simple mixing. This combination led to the self-assembly of a nanostructured fibrillar network of collagen that was ionically linked to the surrounding zwitterionic hydrogel matrix, leading to a composite microstructure reminiscent of soft biological tissues. The addition of 5-15 mg mL-1 collagen and the formation of nanostructured fibrils increased the elastic modulus of the composite system by 40% compared to the base zwitterionic matrix. Most notably, the addition of collagen increased the fracture energy nearly 11-fold ([Formula: see text] 180 J m-2) and clearly delayed crack initiation and propagation. These composites exhibit elastic modulus ([Formula: see text] 0.180 MJ) and toughness ([Formula: see text]0.617 MJ m-3) approaching that of biological tissues such as articular cartilage. Maintenance of the fibrillar structure of collagen also greatly enhanced cytocompatibility, improving cell adhesion more than 100-fold with >90% cell viability.

A pressure-resistant zwitterionic skin sensor for domestic real-time monitoring and pro-healing of pressure injury

Pressure injury (PI) is a hard-to-heal wound to patients with the limited mobility, especially paralyzed or elderly persons. These patients also commonly suffer from sensation loss or dementia that is unable to indicate symptoms in time, resulting in missing the “golden period” for treatment. Therefore, it is highly required to domestic continously real-time monitoring as well as promoting wound healing of PI. However, no existing device has realized these functions for PI. Herein, we prepare a zwitterionic skin sensor that enables pro-healing as well as domestic real-time monitoring the multi-indicators of PI. To apply for a PI dressing that requires to tolerate patient body weight, organosilicon nanoparticles (OSNPs) are designed as crosslinks in the zwitterionic conductive hydrogel (CH-OSNP), which exhibits pressure-resistant properties (99.81% compression to recovery) as well as anti-bacterial adhesion. Moreover, the CH-OSNP-based skin sensor is developed, and the resultant sensor can be sensitive to stress stimuli even under a long-term constant heavy load, which stimulates the pressure of a PI person lying down. In vivo results show that this sensor can not only promote PI healing, but also continuously monitor and distinguish multiple information, such as exudate, swelling, and infection, to prevent PI from being worsen. This work provides a domestic feasible device to cure and monitor the PI of patients.

Zwitterionic Polypeptoids: A Promising Class of Antifouling Bioinspired Materials.

Biofouling caused by protein adsorption and microbial colonization remains a great challenge in many applications. In this work, we synthesized a new type of zwitterionic polypeptoid containing carboxybetaine (CB) moieties (PeptoidCB) through thiol–ene chemistry of poly(N-allylglycine) (PNAG). The zwitterionic antifouling hydrogel was subsequently prepared by co-mixing PeptoidCB with agarose, which exhibited excellent resistance to non-specific protein adsorption and bacterial adhesion. Further, PeptoidCB-modified block copolypeptoids with amphiphilic structure were synthesized to form nanoparticles in an aqueous solution with neglected protein adsorption. The ability of PeptoidCB to resist non-specific protein adsorption and bacterial adhesion makes it a promising candidate for biomedical and industrial applications.

Zwitterionic functionalized catalytic evaporator enables simultaneous solar distillation and organic pollutant degradation

Solar distillation is regarded as a nearly ideal sustainable technology for clean water generation. However, micro- and macro-foulers live in the natural water and volatile organic compounds induced by overdischarging of wastewater are still the main challenges of solar distillation. Herein, a compositive strategy is presented to fabricate self-floatable catalytic evaporators with both solar distillation and organic pollutant degradation, through Fe MOF-loaded electrospinning and antibiofouling zwitterionic coating. The obtained catalytic evaporator with a fibrous structure can lead to enhanced solar distillation rate (1.43 kg m-2h−1) and conversion efficiency (89.41%). More importantly, the zwitterionic hydrogel coating endows the evaporator with superhydrophilicity for continuous water pumping and fascinating multi-contamination repellence against bacteria, alga, oil and salt, and the Fe MOF enables organic pollutants decomposition via photo-Fenton reaction. The currently designed catalytic evaporator integrates the above merits and is expected to provide a new dimension for the designing of multifunctional solar evaporation devices, solving the device contamination and organic residue issues in water treatment.

High voltage and self-healing zwitterionic double-network hydrogels as electrolyte for zinc-ion hybrid supercapacitor/battery

The hydrogel electrolyte is an important part of safety and development potential in zinc-based energy storage equipment due to its inherent low mechanical strength and voltage decomposition. However, hydrogel electrolytes possess a reduced working life for zinc dendrites growth and a narrow voltage window. In this study, a hydrogel electrolyte prepares by the zwitterionic monomer [2-(methacryloyloxy)ethyl]dimethyl-(3-sulfopropyl) (MS) and sodium alginate (SA) alleviate these problems. The zwitterionic double-network hydrogel has good mechanical strength, inhibits the growth of zinc dendrites, enhances practicability, greatly increases the voltage window (0–2.4 V), and has self-healing properties to its rich functional groups. The assembled zinc-ion hybrid supercapacitors (ZHSs) have a high-power density of 172.33 W kg−1 and an energy density of 88.56 Wh·kg−1 at 0.5 A g−1. The assembled zinc-ion battery also has good electrochemical performance. Flexible ZHSs and batteries provide power to the timer stably under different bending angles. The zwitterionic double-network hydrogel can be applied to both zinc-based supercapacitors and batteries.

Anti‐Freezing Self‐Adhesive Self‐Healing Degradable Touch Panel with Ultra‐Stretchable Performance Based on Transparent Triboelectric Nanogenerators

AbstractThe development of next‐generation touch panels requires sensors that are highly sensitive, biocompatible, transparent, stretchable, self‐healing, and even anti‐freezing and self‐powered because the traditional touch panel based on stiff and brittle electrodes faces many challenges. Conductive hydrogels hold great promise as sensing materials for the new‐generation touch panel. However, most hydrogel‐based touch panels are developed based on single‐function gel materials with a lack of the anti‐freezing and self‐power capabilities. Herein, the authors demonstrate a multi‐functional surface‐capacitive touch panel based on a triboelectric nanogenerator with an instantaneous peak power density of 209 mW m−2 that uses zwitterionic network hydrogels as a highly transparent (98.1% transmittance), ultra‐stretchable (&gt;11 500% strain), degradable, and flexible ionic conductor. The panel can be utilized as a human‐machine interactive interface with fast response, high resolution, low parasitic capacitance, functional recovery instantly upon damage, and without sacrificing its functionalities even in the high stretch state (1600% areal strain) and at the subzero environment (&lt;−20 °C). Epidermal touch panels are operated on arbitrary and complex surfaces, with outstanding input property demonstrated by writing, and playing computer games. Simultaneously, the multifunctional touch panel is degradable in phosphate buffered saline solution, and no pollution is caused.

A Self-Association Cross-Linked conductive zwitterionic hydrogel as a myocardial patch for restoring cardiac function

In recent years, engineered cardiac patch (ECP) with electrical conductivity has been developed for cardiac repair after injury or infarction. However, the application of traditional conductive polymers in ECP is still limited due to their toxicity and difficulty in dispersing and degradation. Herein, a self-association crosslinked conductive zwitterionic hydrogel was developed by simple copolymerization of zwitterionic monomer carboxybetaine methacrylate (CBMA) and a biocompatible monomer hydroxyethyl methacrylate (HEMA). The fabricated p(CBMA-co-HEMA) hydrogel possessed excellent ionic conductivity, suitable compressive and stretchable properties, self-healing and mechanical sensory capability. In vitro, the zwitterionic hydrogel significantly enhanced the functionalization of the cardiomyocytes, resulting in excellent synchronous contraction by increasing the expression of cardiac-related factor α-actinin and transmission electrical signal-relevant Connexin-43 (CX-43). In vivo, the hydrogel-derived functional patch effectively promoted the transmission of electrophysiological signals, improved revascularization in infarcted area and then remarkably restored the cardiac function. These data indicated that our developed conductive zwitterionic hydrogel has good promise in repairing myocardial tissue injury.

A Soft Zwitterionic Hydrogel as Potential Coating on a Polyimide Surface to Reduce Foreign Body Reaction to Intraneural Electrodes.

Invasive intraneural electrodes can control advanced neural-interfaced prostheses in human amputees. Nevertheless, in chronic implants, the progressive formation of a fibrotic capsule can gradually isolate the electrode surface from the surrounding tissue leading to loss of functionality. This is due to a nonspecific inflammatory response called foreign-body reaction (FBR). The commonly used poly(ethylene glycol) (PEG)-based low-fouling coatings of implantable devices can be easily encapsulated and are susceptible to oxidative damage in long-term in vivo applications. Recently, sulfobetaine-based zwitterionic hydrogels have emerged as an important class of robust ultra-low fouling biomaterials, holding great potential to mitigate FBR. The aim of this proof-of-principle in vitro work was to assess whether the organic zwitterionic—poly(sulfobetaine methacrylate) [poly(SBMA)]—hydrogel could be a suitable coating for Polyimide (PI)-based intraneural electrodes to reduce FBR. We first synthesized and analyzed the hydrogel through a mechanical characterization (i.e., Young’s modulus). Then, we demonstrated reduced adhesion and activation of fibrogenic and pro-inflammatory cells (i.e., human myofibroblasts and macrophages) on the hydrogel compared with PEG-coated and polystyrene surfaces using cell viability assays, confocal fluorescence microscopy and high-content analysis of oxidative stress production. Interestingly, we successfully coated PI surfaces with a thin film of the hydrogel through covalent bond and demonstrated its high hydrophilicity via water contact angle measurement. Importantly, we showed the long-term release of an anti-fibrotic drug (i.e., Everolimus) from the hydrogel. Because of the low stiffness, biocompatibility, high hydration and ultra-low fouling characteristics, our zwitterionic hydrogel could be envisioned as long-term diffusion-based delivery system for slow and controlled anti-inflammatory and anti-fibrotic drug release in vivo.

Antifreezing zwitterionic hydrogel electrolyte with high conductivity at subzero temperature for flexible sensor and supercapacitor

The presence of large amounts of water in hydrogel electrolyte makes it inevitable freezing at low temperatures, causing it to lose properties such as flexibility or electrical conductivity. It restricts the application of hydrogel electrolyte in subzero temperatures. Here, an antifreezing hydrogel electrolyte is designed and prepared by using zwitterionic and the hydrophilic monomer. The introduction of ethylene glycol (EG) into the hydrogel results in improving the mechanical properties of the hydrogel due to the interaction between EG and the polymer chain. The addition of LiCl not only makes the hydrogel conductive but also enhances the antifreezing and anti-drying properties of the hydrogel, which made the hydrogel exhibit a high ionic conductivity of 1.84 mS cm−1 at −30 °C. The great mechanical properties and electrical conductivity of hydrogels lead to excellent responsiveness in temperature and strain at both ambient and low temperatures. In addition, the electrolyte assembled supercapacitors can be operated normally at low and high temperatures, and their specific capacitance at 60 °C and −20 °C is 108.0% and 48.8% of that at room temperature, respectively.