Engineering Dynamic Hydrophobic Domains in Bioreinforced Ionic Hydrogels for Robust and Transparent Soft Electronics

Conductive hydrogels are attractive platforms for soft electronic materials; however, many high-performance systems rely on conductive fillers, complex multinetwork architectures, or multistep processing that compromise scalability and structural clarity. Here, we report a bioreinforced, filler-free ionic hydrogel engineered through micelle-mediated dynamic hydrophobic domains within a hydrogen-bonded polymer network. Stearyl methacrylate is incorporated into a poly(acrylamide) matrix via SDS-assisted micellization, while gelatin serves as a renewable macromolecular reinforcement, establishing a cooperative network governed by reversible hydrophobic associations and extensive hydrogen bonding. This structure-guided design enables efficient energy dissipation and rapid elastic recovery without permanent structural damage. The optimized hydrogel exhibits ultrahigh stretchability (2420%), enhanced fracture stress (0.31 MPa), high optical transparency (∼85.9%), and low mechanical hysteresis, while maintaining stable ionic conductivity through NaCl incorporation. The dynamic network architecture supports reliable electromechanical response over a wide strain range (0.5-650%), with a maximum gauge factor of 12.08, fast response/recovery times, and excellent cyclic durability. Beyond device-level performance, this work demonstrates how controlled micelle-mediated hydrophobic domain engineering in a bioreinforced polymer matrix can generate mechanically robust, transparent, and conductive soft materials without nanofillers or complex processing. The straightforward one-pot synthesis and use of low-cost components highlight the scalability of this platform for next-generation soft electronic and wearable systems.