A Mechanically Adaptive Aerogel With Active‐Passive Synergistic Cooling

ABSTRACT Passive radiative cooling (PRC) provides an energy‐free route for thermal management but suffers significant performance degradation under humid or cloudy conditions owing to the reduced transparency of the atmospheric window. Herein, a mechanically adaptive sliding‐ring supramolecular aerogel (PCD@PEG/CNF) is developed to integrate passive radiative cooling with molecularly regulated active heat absorption. The aerogel is constructed from poly‐β‐cyclodextrin (PCD) rings and polyethylene glycol (PEG) chains, which form mechanically interlocked host‐guest complexes with mobile junctions that enable reversible molecular motion and continuous enthalpy buffering. This dynamic molecular behavior creates an adaptive heat‐dissipation pathway that synergistically complements passive radiative cooling, resulting in robust and humidity‐resilient cooling performance. Under high solar irradiance and high relative humidity (821.4 W m −2 , 86% RH), the aerogel achieves a sub‐ambient temperature reduction of up to 15.9°C. Experimental and theoretical analyses further reveal that the mobility of the interlocked PCD rings governs the reversible energy‐dissipation process, enabling sustained cooling even when radiative efficiency is restricted. Prepared entirely via a water‐based, and bio‐derived assembly process, this work demonstrates a sustainable strategy for integrating mechanically interlocked molecular dynamics with radiative cooling, offering a promising materials platform for practical thermal management in humid climates.