High‐Toughness and High‐Strength Solvent‐Free Linear Poly(ionic liquid) Elastomers

Abstract Solvent‐free elastomers, unlike gels, do not suffer from solvent evaporation and leakage in practical applications. However, it is challenging to realize the preparation of high‐toughness (with both high stress and strain) ionic elastomers. Herein, high‐toughness linear poly(ionic liquid) (PIL) elastomers are constructed via supramolecular ionic networks formed by the polymerization of halometallate ionic liquid (IL) monomers, without any chemical crosslinking. The obtained linear PIL elastomers exhibit high strength (16.5 MPa), Young's modulus (157.49 MPa), toughness (130.31 MJ m⁻³), and high crack propagation insensitivity (fracture energy 243.37 kJ m⁻²), owing to the enhanced intermolecular noncovalent interactions of PIL chains. Furthermore, PIL elastomer‐based strain, pressure, and touch sensors have shown high sensitivity. The linear noncovalent crosslinked network endows the PIL elastomers with self‐healing and recyclable properties, and broad application prospects in the fields of flexible sensor devices, health monitoring, and human–machine interaction.