A Mimosa‐Inspired Multifunctional Ionogel with Tunable Microphase Separation for High Strength, Shape Memory, and Sensing

ABSTRACT The development of multifunctional ionogels for flexible ionotronics is often hampered by the trade‐off between mechanical robustness and the integration of stimuli‐responsive functionalities. Drawing functional inspiration from the stimulus‐deformation‐signal transduction cascade of Mimosa pudica, we report a liquid crystal‐based click ionogel with a tunable microphase separation that simultaneously achieves high strength, shape memory, and ionic conductivity. This architecture, comprising rigid poly(liquid crystal) domains as the incompatible phase and a soft poly(ionic liquid) network as the compatible matrix, not only reinforces the ionogel (tensile strength >3 MPa, elongation >300%) but also endows it with both shape‐memory and sensing capabilities. The resulting ionogel enables high‐precision flexible sensing across a wide range of deformations, from large‐scale motions to subtle physiological signals. Furthermore, we demonstrate a biomimetic, temperature‐controlled switch that leverages the ionogel's thermally triggered deformation to actuate an alarm circuit, showcasing its potential in intelligent ionotronic devices. This phase‐engineering strategy provides a pathway to circumvent performance trade‐offs in the design of next‐generation soft materials.