Supramolecular Photonic Elastomers with Brilliant Structural Colors and Broad‐Spectrum Responsiveness

Abstract Photonic elastomers (PEs) that can tune their colors through adjusting the lattice spacing of incorporated colloidal particles during mechanical deformation have shown great promise in visualized strain/stress sensors. However, the unsatisfactory structural color and narrow‐spectrum responsiveness limit their broad applications. Herein, carbon‐coated Fe 3 O 4 nanoparticles (Fe 3 O 4 @C NPs) with a high refractive index (RI) and broad light absorption are employed for the construction of PEs with brilliant colors and broad‐spectrum responsiveness by incorporating the Fe 3 O 4 @C NPs into amino‐terminated poly(dimethylsiloxane) (amino‐PDMS) polymer through supramolecular interactions. The inherent light‐absorbing property, high RI, and supramolecular‐induced short‐range ordered arrangement of Fe 3 O 4 @C NPs imparts the PEs with brilliant and angle‐independent structural color. By optimizing the content of Fe 3 O 4 @C NPs in the PEs, broad‐spectrum responsiveness (stopband shifting ≈223 nm) and excellent recovery properties under a large strain can be achieved. The dynamic and reversible interaction endows the PEs with a healable capability. More interestingly, the incorporated Fe 3 O 4 @C NPs with photothermal capability can effectively absorb light and convert it into heat under light irradiation (solar light or near‐infrared laser), accelerating healing of the damaged PEs. This study provides a new strategy for bioinspired construction of PEs for applications in the fields of sensing, colorful coating, and display.