Self‐Adaptable Ternary Eutectic Organogels with Ultrafast Gelation and High Resilience for Multimodal Sensing Coordination

ABSTRACT Flexible sensors that mimic human skin's tactile perception could replace humans in high‐risk tasks. Yet, current materials often suffer performance deterioration in harsh temperatures. While deep eutectic solvents (DESs)‐based polymer networks withstand extreme temperature, creating eutectic organogels that cure controllably and remain highly resilient remains a challenge. This study presents a novel ternary deep eutectic solvent organogel engineered via a competitive solvation strategy. By integrating boric acid into a polyacrylamide network and a glycerol/choline chloride‐based DES, the system utilizes competitive dynamic interactions to effectively minimize the interaction between the solvent and the solute. This design achieves ultrafast (3 s) and broadly tunable (3–180 s) gelation, exhibits exceptional resilience (∼102% strain recovery after 500% stretching, λ res‐3min‐intervel = 6.72%). Furthermore, this material possesses strong adhesiveness, wide temperature adaptability (−80°C to 90°C), superior conductivity (0.368 S m −1 ) and high temperature sensitivity (TCR = 1.886%°C −1 ). These superior comprehensive properties allow it to maintain conformal contact with objects and perform dual‐modal sensing of strain and temperatures. The response curve shows negligible electrical hysteresis, providing consistent output signals at the fixed strain. This work highlights the potential of this gel for applications in human health monitoring and human‐machine interaction.