Cu nanowires (NWs) possess remarkable potential a slow-cost heat transfer material in modern electronic devices. However, Cu NWs with high aspect ratios undergo surface oxidation, resulting in performance degradation. A growth temperature of approximately <1000 °C is required for preventing the changing of Cu NW morphology by the melting of Cu NWs at over 1000 °C. In addition, nitrogen (N)-doped carbon materials coated on Cu NWs need the formation hindrance of oxides and high thermal conductivity of Cu NWs. Therefore, we investigated the N-doped graphene-coated Cu NWs (NG/Cu NWs) to enhance both the thermal conductivity and oxidation stability of Cu NWs. The Cu NWs were synthesized through an aqueous method, and ethylenediamine with an amine group induced the isotropic growth of Cu to produce Cu NWs. At that time, the amine group could be used as a growth source for the N-doped graphene on Cu NWs. To grow an N-doped graphene without changing the morphology of Cu NWs, we report a double-zone growth process at a low growth temperature of approximately 600 °C. Thermal-interface material measurements were conducted on the NG/Cu NWs to confirm their applicability as heat transfer materials. Our results show that the synthesis technology of N-doped graphene on Cu NWs could promote future research and applications of thermal interface materials in air-stable flexible electronic devices.