Multiscale Porous Architecture Consisting of Graphene Aerogels and Metastructures Enabling Robust Thermal and Mechanical Functionalities of Phase Change Materials

Abstract Passive thermal energy storage systems using phase change materials (PCMs) are promising for resolving temporal‐spatial overheating issues from small‐ to large‐scale platforms, yet their poor shape stability due to solid–liquid transition incurs PCM leakage and weak resistance against mechanical disturbance, limiting practical applications. While foam‐stable templates for PCMs have shown complement, they reveal massive leakage and collapse of liquefied PCMs under external loads or impacts. Herein, a multiscale porous architecture consisting of graphene aerogels (GAs) and meta structures enabling robust thermal‐mechanical functionalities of PCMs (3D‐MPGA) toward sustainable phase change thermal energy storage composites is reported. 3D‐printed mechanical metamaterials employing octet‐truss cells provide supportive strength and directionally‐assisted leakage reduction, while GAs serve as porous templates with surface‐interfacial contacts, thereby fixing paraffin wax as PCM inside their nano/micropores. The 3D‐MPGA shows intrinsic thermal characteristics of bulk PCMs, and improved thermal‐mechanical‐chemical stability, confirmed by long‐term heating‐cooling cycle tests over 10 h. Moreover, it exhibits highly reinforced strength (200–5000%) within a low density across ambient and melting temperatures, and maintains original shapes in the liquefied PCMs without severe leakage, against external loads. This work inspires rational strategies for advancing robust thermal‐mechanical functionalities for PCM‐based thermal energy storage systems.