▎ 摘　　要

Graphene-based papers have recently triggered considerable interests in developing the application as thermal interface materials (TIMs) for addressing the interfacial heat transfer issue, but their low through-plane thermal conductivity (kappa perpendicular to), resulting from the layer-by-layer stacked architecture, limits the direct use as TIMs. Although various hybrid graphene papers prepared by combining the graphene sheets and the thermally conductive insertions have been proposed to solve this problem, achieving a satisfactory kappa perpendicular to higher than that of commercial TIMs (>5 W m-1 K-1) remains challenging. Here, a strategy aimed at the construction of heat pathways along the through-plane direction inside the graphene paper for achieving a high kappa perpendicular to was demonstrated through the simultaneous filtration of graphene sheets with two different lateral sizes. The as-prepared graphene paper presented a hierarchical structure composed of loosely stacked horizontal layers formed by large graphene sheets, intercalated by a random arrangement of small graphene sheets. Due to the heat pathways formed by small graphene sheets along the through-plane direction, the hierarchically structured graphene paper exhibited an improved kappa perpendicular to as high as 12.6 W m-1 K-1 after a common graphitization post-treatment. In the practical test, our proposed paper as an all-graphene TIM achieved an enhancement in cooling efficiency of approximate to 2.2 times compared to that of the state-of-the-art TIM, demonstrating its superior performance to meet the ever-increasing heat dissipation requirement.