A Microphase‐Separated Design toward an All‐Round Ionic Hydrogel with Discriminable and Anti‐Disturbance Multisensory Functions

Abstract Stretchable ionic hydrogels with superior all‐round properties that can detect multimodal sensations with excellent discriminability and robustness against external disturbances are highly required for artificial electronic skinapplications. However, some critical material parameters exhibit intrinsic tradeoffs with each other for most ionic hydrogels. Here, a microphase‐separated hydrogel is demonstrated by combining three strategies: (1) using of a low crosslinker/monomer ratio to obtain highly entangled polymer chains as the first network; (2) the introduction of zwitterions into the first network; (3) the synthesis of an ultrasoft polyelectrolyte as the second network. This all‐round elastic ionic hydrogel exhibits a low Young's modulus (< 60 kPa), large stretchability (> 900%), high resilience (> 95%), unique strain‐stiffening behavior, excellent fatigue tolerance, high ionic conductivity (> 2.0 S m⁻¹), and anti‐freezing capability, which have not been achieved before. These properties allow the ionic hydrogel to operate as a stretchable multimodal sensor that can detect and decouple multiple stimuli (temperature, pressure, and proximity) with excellent discriminability, high sensitivity, and strong sensing‐robustness against strains or temperature perturbations. The ionic hydrogel sensor exhibits great potential for intelligent electronic skin applications such as reliable health monitoring and accurate object identification.