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.