Tourmaline/graphene oxide (TGOx, x = 5, 10, 15, and 20) compound with high thermal conductivity and high far infrared emissivity was prepared by a refluxing method. Transmission electron microscopy results confirmed that graphene oxide with a few layers was fabricated, and tourmaline nanoparticles were supported by graphene oxide layers. Thermal interface materials were prepared by adding tourmaline/graphene oxidex compound into epoxy resin. Far infrared emissivity of TGOx and thermal conductivity of thermal interface materials were increased with the weight ratio of graphene oxide in compound, but the corresponding electrical conductivity was slightly decreased. In particular, the tourmaline/graphene oxide15 (tourmaline/graphene oxide ratio of 85:15) showed an enhancement of 4% in far infrared emission than that of tourmaline. The thermal conductivity of thermal interface materials with 5 wt% tourmaline/graphene oxide15 was improved by 380% compared with that of pure epoxy resin, and the electrical conductivity of tourmaline/graphene oxide/epoxy was decreased slightly compared to that of graphene oxide/epoxy.