Supramolecularly Connected Armor-like Nanostructure Enables Mechanically Robust Radiative Cooling Materials

Passive daytime radiative cooling (PDRC) is a promising practice to realize sustainable thermal management with no energy and resources consumption. However, there remains a challenge of simultaneously integrating desired solar reflectivity, environmental durability, and mechanical robustness for polymeric composites with nanophotonic structures. Herein, inspired by a classical armor shell of a pangolin, we adopt a generic design strategy that harnesses supramolecular bonds between the TiO₂-decorated mica microplates and cellulose nanofibers to collectively produce strong interfacial interactions for fabricating interlayer nanostructured PDRC materials. Owing to the strong light scattering excited by hierarchical nanophotonic structures, the bioinspired film demonstrates a desired reflectivity (92%) and emissivity (91%) and an excellent temperature drop of 10 °C under direct sunlight. Notably, the film guarantees high strength (41.7 MPa), toughness (10.4 MJ m^-3), and excellent environmental durability. This strategy provides possibilities in designing polymeric PDRC materials, further establishing a blueprint for other functional applications like soft robots, wearable devices, etc.