Abstract: In order to prepare graphite/Cu composites with excellent thermodynamic properties, the natural graphite flakes were highly oriented on the surface of copper foil by tape casting method. The high-oriented graphite flake/Cu composites with layered structure were prepared by vacuum hot-pressing method. The phases and morphology of graphite flake/Cu composites were characterized by XRD and SEM. The results show that the solvent used for casting is fully volatilized after heat-treated process. The aligned graphite flakes between two copper foil layers overlap each other and partially melted copper penetrates other copper layers across the pores of the graphite layer. This structure allows the graphite/Cu composite to achieve excellent thermophysical properties. As the volume fraction of graphite is 20vol% to 70vol%, the thermal conductivity of the graphite flake/Cu composite increases from 402 W/(m·K) to 743 W/(m·K) in high thermal conductivity plane, while the bending strength is 126~48 MPa.The heat transfer mechanism of graphite flake/Cu composites is discussed deeply and a thermal conductivity prediction model has been established.