It is essential and of great significance to impart high mechanical performance, environmental stability, and high sensitivity to emerging flexible temperature sensors. In this work, polymerizable deep eutectic solvents are designed and prepared by simply mixing N‐cyanomethyl acrylamide (NCMA) containing an amide group and a cyano group in the same side chain with lithium bis(trifluoromethane) sulfonimide (LiTFSI), and obtain supramolecular deep eutectic polyNCMA/LiTFSI gels after polymerization. These supramolecular gels exhibit excellent mechanical performance (tensile strength of 12.9 MPa and fracture energy of 45.3 kJ m−2), strong adhesion force, high‐temperature responsiveness, self‐healing ability, and shape memory behavior due to the reversible reconstruction ability of amide hydrogen bonds and cyano‐cyano dipole‐dipole interactions in the gel network. In addition, the gels also demonstrate good environmental stability and 3D printability. To verify its application potential as a flexible temperature sensor, the polyNCMA/LiTFSI gel‐based wireless temperature monitor is developed and displays outstanding thermal sensitivity (8.4%/K) over a wide detection range. The preliminary result also suggests the promising potential of PNCMA gel as a pressure sensor.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.