<p>Flexible photonic crystal (PC) materials possess exceptional optical properties. However, their structures often deteriorate under repeated mechanical responses, which may lead to structural impairments within the photonic band gap. This poses a challenge to their sustainability. Herein, by introducing a self-healing thermoplastic polyurethane (STPU) material with inverse-opal PC structure, a self-healing discoloration skin with stress response is prepared, inspired by the structural coloration and self-healing mechanisms of natural organisms. Given the synergistic effects of dynamic covalent bonds (S-S bonds) and hydrogen bonds (H-bonds), STPU can be reversibly adjusted upon mechanical deformation, enabling it to coordinate with environmental changes and showing excellent mechanical strength (26.76 MPa) and elongation at break (2000%). At the same time, the inverse opal structure inside STPU gives composite reversible color transitions with sensitive optical responses to solvents (e.g., water and ethanol) and mechanical stress (0%–70% strain) through the regulation of lattice spacing. Furthermore, the incorporation of an interpenetrating network composed of polyacrylamide hydrogel and carbon nanotubes enhances its strain sensitivity and structural color stability. More importantly, given its excellent self-healing properties, it exhibits broad application potential in flexible sensors, adaptive optical devices, bioinspired robotic skins, and dynamic anticounterfeiting encryption, overcoming the limitations of traditional PCs (e.g., high fragility and single functionality). The proposed strategy paves the way for the development of durable intelligent sensing materials with enhanced environmental adaptability and multifunctional integration.</p>