| Summary: | Ionic conductive hydrogels with good conductivity and biocompatibility have become one of the research highlights in the field of wearable flexible sensors and supercapacitors. In this work, poly(methacrylic acid–methyl methacrylate)-reinforced poly(sodium acrylate–vinyl phosphonic acid) composite hydrogels (P(AAS-VPA)/PMMS) were designed and tested for strain sensor or supercapacitor applications. The results showed recoverability for 20 cycles of tension and compression experiments, an excellent breaking strain of 2079%, and ionic conductivity of 0.045 S·cm<sup>−1</sup>, demonstrating strong support for the application of the P(AAS-VPA)/PMMS hydrogel in strain sensors and supercapacitors. The composite hydrogel exhibited outstanding sensing and monitoring capability with high sensitivity (GF = 4.0). The supercapacitor based on the P(AAS-VPA)/PMMS composite hydrogel showed excellent capacitance performance (area capacitance 100.8 mF·cm<sup>−2</sup> and energy density 8.96 μWh·cm<sup>−2</sup>) at ambient temperature and even −30 °C (25.3 mF·cm<sup>−2</sup> and 2.25 μWh·cm<sup>−2</sup>). The hydrogel has stable electrochemical stability (1000 cycles, Coulomb efficiency > 97%) and exhibits electrochemical properties similar to those in the normal state under different deformations. The excellent results demonstrate the great potential of the P(AAS-VPA)/PMMS composite hydrogel in the field of strain sensors and flexible supercapacitors.
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