Thermal management has become a crucial issue for the rapid development of electronic devices, and thermal interface materials (TIMs) play an important role in improving heat dissipation. Recently, carbon−based TIMs, including graphene, reduced graphene oxide, and carbon nanotubes (CNTs) with high thermal conductivity, have attracted great attention. In this work, we provide graphene−carbon nanotube composite films with improved electrical and thermal conductivities. The composite films were prepared from mixed graphene oxide (GO) and CNT solutions and then were thermally reduced at a temperature greater than 2000 K to form a reduced graphene oxide (rGO)/CNT composite film. The added CNTs connect adjacent graphene layers, increase the interlayer interaction, and block the interlayer slipping of graphene layers, thereby improving the electrical conductivity, through−plane thermal conductivity, and mechanical properties of the rGO/CNT composite film at an appropriate CNT concentration. The rGO/CNT(4:1) composite film has the most desired properties with an electrical conductivity of ~2827 S/cm and an in−plane thermal conductivity of ~627 W/(m·K). The produced rGO/CNT composite film as a TIM will significantly improve the heat dissipation capability and has potential applications in thermal management of electronics.