Multi‐Scenario Adaptive High‐Fidelity Self‐Healing Elastomer Based on Poly(Ionic Liquid) Containing Polyurethane for Temperature‐Pressure Sensing and Human‐Machine Interaction

ABSTRACT Skin‐friendly ionogels with multi‐scenario adaptive, high‐fidelity, and self‐healing performances were critical building units in wearable signal transmission devices. Traditional ionogels doped with small‐molecule ionic liquids (SMILAs) into polymers yielding weak interchain forces, poor compatibility, and migration. To remedy this issue, a kind of polyurethane (PU) based healable ionogel containing polyimidazolium (PIM), adipic acid dihydrazide (ADH), and SMILAs (IL; BMIM:TFSI) was fabricated via continuous chemical copolymerization and physical co‐molding. The PIM/ADH/IL n @PU ( n = 0.1–0.6, representing the content of IL) ionogels exhibited excellent mechanical properties with tensile strength of 10.93 MPa, elongation as high as 1020.23%, ionic conductivity up to 0.45 mS/cm, and an efficient self‐healing ratio of 98.3% in 3 h at 33°C. Moreover, the PIM‐induced low migration of IL without an electric field, outstanding antibacterial activity (over 99% inhibition against E. coli and S. aureus ), superior biocompatibility (over 95% cell viability), sweat and humidity insensitivity, and multiple regenerability were also demonstrated. The strain sensitivity and temperature‐pressure sensing capability endowed these ionogels to be optimized candidates to construct motion monitoring, underwater early warning, and breathing monitoring devices. The realization of the human‐machine interaction model provided a new avenue for flexible wearable sensors and promoted the development of remote mechanical control systems.