Graphene‐Based Ultralight Compartmentalized Isotropic Foams with an Extremely Low Thermal Conductivity of 5.75 mW m−1 K−1

Abstract The importance of high‐performance thermal insulation materials is rapidly emerging due to energy conservation and the management of temperature‐sensitive device perspectives. Recent thermal insulation materials including complex structures have been developed either by reducing the structural connectivity to mitigate thermal transport through solid conduction or forming directionally aligned confined inner pores to suppress the internal gas convection. In this study, to create a highly efficient thermal insulating material that suppresses thermal transport in all directions, graphene‐based anisotropic closed‐cellular structures (CCS) are devised with a highly ordered assembly of hollow compartments with extremely thin walls (≈50 nm). This uniquely designed CCS made from microfluidically synthesized graphene solid bubbles exhibited a remarkably low thermal conductivity of 5.75 mW m −1 K −1 thanks to effective suppression of both solid conduction and gas conduction/convection. Therefore, the proposed strategy in this work offers a novel toolkit for implementing next‐generation high‐performance insulation materials.