Solvent‐Triggered, Ultra‐Adhesive, Conductive, and Biocompatible Transition Gels for Wearable Devices

Abstract The development of robust adhesive, conductive, and flexible materials has garnered significant attention in the realm of human‐machine interface and electronic devices. Conventional preparation methods to achieve these exceptional properties rely on incorporating highly polar raw materials, multiple components, or solvents. However, the overexposure of functional groups and the inherent toxicity of organic solvents often render gels non‐stick or potentially biocompatible making them unsuitable for human‐contact devices. In this study, a straightforward three‐step strategy is devised for preparing responsive adhesive gels without complex components. Structurally conductive poly( N ‐(2‐hydroxyethyl)‐acrylamide‐co‐p‐styrene sulfonate hydrate) (PHEAA‐NaSS) gels are synthesized by integrating ionic and hydrophilic networks with distinct solvent effects. Initially, the in‐suit formed PHEAA‐NaSS networks are activated by dimethyl sulfoxide, which substantially increases intramolecular hydrogen bonding and enhances the matrix stretchability and interfacial adhesion. Subsequently, ethanol exchange reduced solvent impact and led to a compact network that limited surface exposure of ionic and hydrophilic groups, resulting in nonstick, robust for convenient storage. Finally, upon contacting with water, the network demonstrates rehydration, resulting in favorable adhesion, biocompatibility, and conductivity. The proposed PHEAA‐NaSS/W gels can stably and reliably capture joint motion and electrophysiological signals. Furthermore, this uncomplicated gel preparation method is also applicable to other electrolyte monomers.