Sea Cucumber‐Inspired Polyurethane Demonstrating Record‐Breaking Mechanical Properties in Room‐Temperature Self‐Healing Ionogels

Abstract Practical applications of existing self‐healing ionogels are often hindered by the trade‐off between their mechanical robustness, ionic conductivity, and temperature requirements for their self‐healing ability. Herein, this challenge is addressed by drawing inspiration from sea cucumber. A polyurethane containing multiple hydrogen‐bond donors and acceptors is synthesized and used to fabricate room‐temperature self‐healing ionogels with excellent mechanical properties, high ionic conductivity, puncture resistance, and impact resistance. The hard segments of polyurethane, driven by multiple hydrogen bonds, coalesce into hard phase regions, which can efficiently dissipate energy through the reversible disruption and reformation of multiple hydrogen bonds. Consequently, the resulting ionogels exhibit record‐high tensile strength and toughness compared to other room‐temperature self‐healing ionogels. Furthermore, the inherent reversibility of multiple hydrogen bonds within the hard phase regions allows the ionogels to spontaneously and efficiently self‐heal damaged mechanical properties and ionic conductivity multiple times at room temperature. To underscore their application potential, these ionogels are employed as electrolytes in the fabrication of electrochromic devices, which exhibit excellent and stable electrochromic performance, repeatable healing ability, and satisfactory impact resistance. This study presents a novel strategy for the fabrication of ionogels with exceptional mechanical properties and room‐temperature self‐healing capability.