Alkaline‐Responsive, Self‐Healable, and Conductive Copolymer Composites with Enhanced Mechanical Properties Tailored for Wearable Tech

Abstract Despite significant advancements, current self‐healing materials often suffer from a compromise between mechanical robustness and functional performance, particularly in terms of conductivity and responsiveness to environmental stimuli. Addressing this issue, the research introduces a self‐healable and conductive copolymer, poly(ionic liquid‐ co ‐acrylic acid) (PIL‐ co ‐PAA), synthesized through free radical polymerization, and further optimized by incorporating thermoplastic polyurethane (TPU). This combination leverages the unique properties of each component, especially ion‐dipole interactions and hydrogen bonds, resulting in a material that exhibits exceptional self‐healing abilities and demonstrates enhanced mechanical properties and electrical conductivity. Moreover, the PIL‐ co ‐PAA/TPU films showcase alkaline‐responsive behavior, a feature that broadens their applicability in dynamic environments. Through systematic characterization, including thermogravimetric analysis, tensile testing, and electrical properties measurements, the mechanisms behind the improved performance and functionality of these films are elucidated. The conductivities and ultimate tensile strength (σ _uts ) of the PIL‐ co ‐PAA/TPU films regain 80% under 8 h healing process. To extend the applications for wearable devices, the self‐healing properties of commercial cotton fabrics coated with the self‐healable PIL‐ co ‐PAA are also investigated, demonstrating both self‐healing and electrical properties. This study advances the understanding of self‐healable conductive polymers and opens new avenues for their application in wearable technology.