Monomer Trapping Synthesis Toward Dynamic Nanoconfinement Self‐healing Eutectogels for Strain Sensing

Abstract The rapid advancement in attractive platforms such as biomedicine and human‐machine interaction has generated urgent demands for intelligent materials with high strength, flexibility, and self‐healing capabilities. However, existing self‐healing ability materials are challenged by a trade‐off between high strength, low elastic modulus, and healing ability due to the inherent low strength of noncovalent bonding. Here, drawing inspiration from human fibroblasts, a monomer trapping synthesis strategy is presented based on the dissociation and reconfiguration in amphiphilic ionic restrictors (7000‐times volume monomer trapping) to develop a eutectogel. Benefiting from the nanoconfinement and dynamic interfacial interactions, the molecular chain backbone of the formed confined domains is mechanically reinforced while preserving soft movement capabilities. The resulting eutectogels demonstrate superior mechanical properties (1799% and 2753% higher tensile strength and toughness than pure polymerized deep eutectic solvent), excellent self‐healing efficiency (>90%), low tangential modulus (0.367 MPa during the working stage), and the ability to sensitively monitor human activities. This strategy is poised to offer a new perspective for developing high strength, low modulus, and self‐healing wearable electronics tailored to human body motion.