This study focuses on the preparation of stretchable zwitterionic poly(sulfobetaine methacrylate) (PSBMA) hydrogels. To address the weak mechanical properties of chemically crosslinked PSBMA hydrogels, a physical crosslinking method utilizing hydrophobic interactions to crosslink hydrogels to approach tough properties is developed. Here, sodium dodecyl sulfate (SDS)‐based micelle is used as a physical crosslinker to prepare physically crosslinked PSBMA (PSBMAphy) hydrogels, and ethylene glycol dimethylacrylate (EGDMA) is used to prepare a control group of chemically crosslinked PSBMA (PSBMAchem) hydrogels. The mechanical properties of the two hydrogels are compared, and PSBMAphy hydrogels exhibit greater flexibility than the PSBMAchem hydrogels. When the PSBMAphy hydrogels are subjected to external forces, the micelles act as dynamic crosslinking sites, allowing the stress to disperse and prevent the hydrogel from breaking. In addition, the PSBMAphy hydrogels have nearly 100% self‐healing properties within 2.5 min. The PSBMAphy hydrogels exhibit usable adhesive properties to porcine skin and subcutis. MTT and hemolysis tests show that the PSBMAphy hydrogels have excellent biocompatibility and hemocompatibility. This study proposes that the multifunctional PSBMAphy hydrogels with micelles will be potential to carry drugs for use in drug delivery systems in the future.

Poly(2-hydroxyethyl methacrylate) (polyHEMA) hydrogels are commonly used in biomaterials such as contact lenses. However, water evaporation from these hydrogels can cause discomfort to wearers, and the bulk polymerization method used to synthesize them often results in heterogeneous microstructures, reducing their optical properties and elasticity. In this study, we synthesized polyHEMA gels using a deep eutectic solvent (DES) instead of water and compared their properties to traditional hydrogels. Fourier-transform infrared spectroscopy (FTIR) showed that HEMA conversion in DES was faster than in water. DES gels also demonstrated higher transparency, toughness, and conductivity, along with lower dehydration, than hydrogels. The compressive and tensile modulus values of DES gels increased with HEMA concentration. A DES gel with 45% HEMA showed excellent compression–relaxation cycles and had the highest strain at break value in the tensile test. Our findings suggest that DES is a promising alternative to water for synthesizing contact lenses with improved optical and mechanical properties. Furthermore, DES gels’ conduction properties may enable their application in biosensors. This study presents an innovative approach to synthesizing polyHEMA gels and provides insights into their potential applications in the biomaterials field.