Dynamic Disulfide Ionogels for Self‐Healing, Transparent, and Elastic E‐Skins

ABSTRACT Ionogel E‐skins that combine high elasticity, optical transparency, and autonomous self‐healing are highly desirable yet remain challenging to realize owing to the intricate and interdependent physicochemical interactions between polymer networks and ionic liquids. Here, dynamic covalent ionogels, formed by a disulfide–crosslinked tetra‐arm polyethylene glycol network, were systematically engineered by tuning the identity and composition of ionic liquids. We show that polymer–ionic liquid compatibility, viscosity, and ionic liquid content collectively regulate polymer segmental mobility, which governs disulfide exchange kinetics and thereby dictates healing efficiency and elasticity. The optimized ionogel is fully amorphous and exhibits 99% self‐healing at 25°C within 2 h, a low residual strain of 1.7% after a 100% cyclic tensile test, and 93% optical transmittance at 700 nm. As an ionogel electronic skin, it maintains stable sensing under repeated deformation, recovers its initial functionality after complete damage through self‐healing, and enables reliable real‐time strain sensing of the neck, wrist, finger, and knee. These findings establish chain‐mobility engineering as an effective design principle for robust wearable ionogel electronics.