Carbonous nanomaterials are promising additives for composite coatings for heat-dissipation materials because of their excellent thermal conductivity. Here, copper/carbonous nanomaterial composite coatings were prepared using nanodiamond (ND) as the carbonous nanomaterial. The copper/ND composite coatings were electrically deposited onto copper substrates from a continuously stirred copper sulfate coating bath containing NDs. NDs were dispersed by ultrasonic treatment, and the initial bath pH was adjusted by adding sodium hydroxide solution or sulfuric acid solution before electrodeposition. The effects of various coating conditions—the initial ND concentration, initial bath pH, stirring speed, electrical current density, and the amount of electricity—on the ND content of the coatings were investigated. Furthermore, the surface of the NDs was modified by hydrothermal treatment to improve ND incorporation. A higher initial ND concentration and a higher stirring speed increased the ND content of the coatings, whereas a higher initial bath pH and a greater amount of electricity decreased it. The electrical current density showed a minimum ND content at approximately 5 A/dm². Hydrothermal treatment, which introduced carboxyl groups onto the ND surface, improved the ND content of the coatings. A copper/ND composite coating with a maximum of 3.85 mass% ND was obtained.