Biomimetic Mechanically Robust Chiroptical Hydrogel Enabled by Hierarchical Bouligand Structure Engineering.

Natural bouligand structures enable crustacean exoskeletons and fruits to strike a combination of exceptional mechanical robustness and brilliant chiroptical properties owing to multiscale structural hierarchy. However, integrating such a high strength-stiffness-toughness combination and photonic functionalities into synthetic hydrogels still remains a grand challenge. In this work, we report a simple yet general biomimetic strategy to construct an ultrarobust chiroptical hydrogel by closely mimicking the natural bouligand structure at multilength scale. The hierarchical structural engineering of long-range ordered cellulose nanocrystals' bouligand structure, well-defined poly(vinyl alcohol) nanocrystalline domains, and dynamic interfacial interaction synergistically contributes to the integration of high strength (23.3 MPa), superior modulus (264 MPa), and high toughness (54.7 MJ m-3), as well as extraordinary impact resistance, which far exceed their natural counterparts and synthetic photonic hydrogels. More importantly, seamless chiroptical and solvent-responsive patterns with high resolution can also be scalably integrated into the hydrogel by localized manipulation of the photonic band, while maintaining good ionic conductivity. Such exceptional mechanical-photonic combination holds tremendous potential for applications in wearable sensors, encryption, displays, and soft robotics.