Kai Zheng, Jingshen Wu, Linbo Zhang, Xianyu Jiang, Ce Bian
Abstract Polyurethane‐based ionoelastomers possess high ionic conductivity, stretchability, and thermal stability, making them promising candidates for flexible ionotronics. However, conventional polyurethane‐based ionoelastomers are fabricated by blending ionic liquids (ILs) into a polyurethane matrix, which often leads to phase separation due to poor component compatibility. Herein, a covalent integration strategy is reported to synthesize a highly stretchable iPF127‐PU ionoelastomer through direct polymerization of a photopolymerizable IL with polyurethane chains derived from Pluronic F127 (PF127), a triblock polyether. The iPF127‐PU ionoelastomer exhibits ionic conductivity of 1.07 × 10 −4 S m −1 and an elongation at break of up to 450%. When assembled as a flexible sensor, the iPF127‐PU‐based sensor demonstrates an initial sensitivity of 79.8 kPa −1 , a rapid response/recovery speed of 50 ms, and maintains exceptional mechanical stability over 10 000 s static loading. Moreover, it enables steady and precise control in robotic manipulation. This strategy facilitates artificial tactile perception in robotic systems, offering significant potential for advanced intelligent grasping and human‐machine interfaces.