Recently, the amount of heat generated in devices has been increasing due to the miniaturization and high performance of electronic devices. Cu-graphite composites are emerging as a heat sink material, but its capability is limited due to the weak interface bonding between the two materials. To overcome these problems, Cu nanoparticles were deposited on a graphite flake surface by electroless plating to increase the interfacial bonds between Cu and graphite, and then composite materials were consolidated by spark plasma sintering. The Cu content was varied from 20 wt.% to 60 wt.% to investigate the effect of the graphite fraction and microstructure on thermal conductivity of the Cu-graphite composites. The highest thermal conductivity of 692 W m⁻¹K⁻¹ was achieved for the composite with 40 wt.% Cu. The measured coefficients of thermal expansion of the composites ranged from 5.36 × 10⁻⁶ to 3.06 × 10⁻⁶ K⁻¹. We anticipate that the Cu-graphite composites have remarkable potential for heat dissipation applications in energy storage and electronics owing to their high thermal conductivity and low thermal expansion coefficient.