ABSTRACT The development of materials that simultaneously offer broadband electromagnetic protection, optical transparency, mechanical flexibility, and intelligent responsiveness remains a formidable challenge in the advancement of next‐generation smart windows. In this study, a synergistic design strategy that integrates multi‐component molecular engineering with in‐situ microphase separation was introduced, leading to the successful fabrication of a novel multifunctional ionogel. This approach enables the spatial decoupling of the mechanical framework from ion transport and polarization domains within a nanoscale bicontinuous structure, effectively addressing the trade‐off between mechanical strength and ionic conductivity. The optimized ionogel demonstrates an ultra‐wide effective absorption bandwidth of 8.08 GHz at a remarkably thin thickness of 1.72 mm, along with high visible‐light transmittance exceeding 93% and excellent mechanical properties, including a fracture strain of 406%. Furthermore, by incorporating photochromic molecules, the material exhibits light‐gated microwave absorption characteristics with reversible bandwidth tuning and achieves passive radiative cooling exceeding 22.83°C under simulated sunlight. Differential charge density calculations further confirm electron accumulation at the hard/soft phase interfaces, providing atomic‐scale evidence for interfacial polarization. This work establishes a new paradigm of microstructure‐driven molecular design, opening a new avenue for the development of next‐generation electromagnetic protection and thermal management systems.
Wu et al. (2026) studied this question.