▎ 摘　　要

As the power density of electronic devices continuously increases, there is a growing demand to improve the heat conduction performance of thermal management materials for addressing heat dissipation issues. Single-/few-layer graphene is a promising candidate as a filler of a metal matrix due to its extremely high thermal conductivity (k); however, the well arranged assembly of 2D-component graphene with a high volume fraction remains challenging. Herein, we integrated a novel graphene-based macroscopic material of graphene film (GF) into a Cu matrix by infiltrating molten Zr-microalloyed Cu into a spirally folded and upright-standing GFs skeleton. The microstructure of the GF/Cu composites was regulated by an interface modification strategy. The GF/Cu composites with a spirally layered microstructure exhibit a superior k of 820 W/m K in the axial direction, much higher than that of Cu-matrix composites reinforced with graphene nanosheets (generally <500 W/m K) and twice that of Cu. The thermal transfer mechanisms were investigated by experiments and theoretical calculations. The results reveal that the excellent performance is attributed to the construction of high-heat conduction channels and a positive coordinating effect at the Zr-modified GF/Cu interface. Meanwhile, the relation between interfacial microstructure and heat transfer is established in the composites using interfacial thermal resistance as a bridge. This work yields in-depth insight into the heat conduction mechanism in highly oriented structures and provides a promising solution for the thermal management issues of high-power electronics.