Glycerol‐Induced Network Decoupling‐Reconstruction Enables Mechanically Matched and Highly Ion‐Conductive Eutectogels for Skin‐Conformal Strain Sensing

Comprehensive Summary Skin‐conformal strain sensors demand ion‐conductive gels that simultaneously exhibit tissue‐matched softness, large deformability, and efficient signal transduction. However, in conventional eutectogels, the strong covalent/physical coupling that ensures network stability simultaneously stiffens the polymer matrix and confines ion migration, causing an intrinsic conflict between mechanical compliance and ionic conductivity. Herein, we propose a glycerol‐induced network decoupling‐reconstruction strategy to simultaneously regulate mechanical properties and ionic conductivity in choline chloride/polyacrylic acid eutectogels. Glycerol competitively weakens interchain hydrogen bond and ion‐polymer interactions through the hydrogen bond and solvation effects, while reconstructing a dynamic network with enhanced chain mobility and continuous ion‐conduction pathways. The optimized eutectogel exhibits a skin‐matched Young's modulus of 277.23 kPa, elongation at break of 1379.43%, tensile strength of 225.89 kPa, toughness of 2.11 MJ·m –3 , and ionic conductivity of 0.26 S·m –1 . Benefiting from this synergistic optimization of mechanical and ionic properties, the eutectogel strain sensor shows broad‐range sensing, good sensitivity, fast response, and stable cycling performance. Moreover, it enables wireless monitoring of subtle physiological signals, joint motions, and multichannel gestures, demonstrating its promise as a next‐generation platform for wearable ionotronic devices.