Zn ² ⁺ ‐Mediated Densification of Amorphous Network in Ternary Eutectogel for Wireless Assistive Monitoring

ABSTRACT The trade‐off between mechanical robustness and ionic conductivity in gel materials impedes their application in flexible electronics. Herein, a eutectogel is engineered via a synergistic strategy that integrates a ternary deep eutectic solvent (DES) (choline chloride/ethylene glycol/zinc chloride) with dynamic Zn 2 + coordination. Through in situ photopolymerization of 1‐vinylimidazole in the ternary DES, a dynamically cross‐linked organic‐inorganic hybrid network is constructed. Crucially, Zn 2 + ions play a dual role: they form reversible Zn 2 + –imidazole coordination sites, enhancing the mechanical properties with an elongation at break of 1100% and a Young's modulus of 0.23 MPa, while inducing coordination‐driven densification of the amorphous network. This compaction effect tightens the polymer network without triggering crystallization, while accessible ion‐transport pathways are retained within the amorphous network. Consequently, the eutectogel exhibits a high ionic conductivity of 0.38 mS cm − 1 , overcoming the typical conductivity loss in high‐strength gels. Using these properties, a flexible strain‐sensing system with Bluetooth transmission is developed. It can capture real‐time motor signals and convert them into visual commands, highlighting its potential for wireless assistive monitoring, particularly in rehabilitation for hemiplegic patients. This work provides a promising strategy for achieving a balance between mechanical robustness and ionic conductivity in soft materials by regulating the amorphous structure.