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Passive daytime radiation cooling (PDRC) has gained considerable attention as an emerging and promising cooling technology. Polymer‐based porous materials are one of the important candidates for PDRC application due to their easy processing, free of inorganic particle doping, and multifunctionality. However, the mechanical properties of these porous materials, which are critical in outdoor services, have been overlooked in previous studies. Herein, a nonsolvent‐induced phase separation (NIPS) method combined with ambient pressure drying to prepare polyethylene‐polysilicate all‐polymer porous coatings is developed. The coatings possess a Cyphochilus beetle‐like skeleton structure with optimal skeleton size, laminated anisotropy, and high volume fraction (64 ± 1%). These structure features ensure a maximum skeleton density without optical crowding, thus enhancing light scattering and stress dispersion, and balancing optical and mechanical properties. The coatings exhibit significant mechanical robustness (only ≈70 µm thickness reduction after 1000 Taber abrasion cycles at a 750 g load without influencing optical performance), durability, optical properties (a solar reflectance of ≈95% and an average near‐normal thermal emittance of ≈96%), and PDRC performance (realizing sub‐ambient cooling of ≈3–6 °C at midday with different weather conditions). The work provides a new solution to improve the practicability of polymer‐based porous coatings in PDRC outdoor services and other fields. [ABSTRACT FROM AUTHOR]

The scales of the white Cyphochilus beetles are endowed with unusual whiteness arising from the exceptional scattering efficiency of their disordered ultrastructure optimized through millions of years of evolution. Here, a simple, one‐step method based on water vapor–induced phase separation is developed to prepare thin polystyrene films with similar microstructure and comparable optical performance. A typical biomimetic 3.5 µm PS film exhibits a diffuse reflectance of 61% at 500 nm wavelength, which translates into a transport mean free path below 1 µm. A complete optical characterization through Monte Carlo simulations reveals how such a scattering performance arises from the scattering coefficient and scattering anisotropy, whose interplay provides insight into the morphological properties of the material. The potential of bright‐white coatings as smart sensors or wearable devices is highlighted using a treated 3.5 µm film as a real‐time sensor for human exhalation. [ABSTRACT FROM AUTHOR]