A new ternary solid solution, Cu3-xNix+yN, is prepared by gas-pulsed CVD at 260 °C. Gas pulses of the precursor mixtures Cu(hfac)2 + NH3 and Ni(thd)2 + NH3, separated by intermittent ammonia pulses, are employed for the deposition of Cu3N and Ni3N, respectively. A few monolayers of the nitrides are grown in each CVD pulse and then mixed by diffusion to produce the solid solution. The metal content of the solid solution can be varied continuously from 100% to about 20% Cu, which means that the electrical properties can be varied from 1.6 eV (band gap of Cu3N) to metallic (Ni3N). This is of interest for various applications, e.g., solar energy, catalysis, and microelectronics.