Single phase solid solutions based on copper and iron substitution into the nickel sites of Ni2Mo3N are produced using a citrate gel approach followed by ammonolysis. These metal nitrides show good ammonia synthesis activity at 500 °C and ambient pressure. The activity fell with copper content and increased with iron content, although these changes appear to be related to the surface areas of the catalysts. The oxide intermediates from the citrate gel process cleanly converted to the metal nitride under the ammonia synthesis gas stream (75% H2, 25% N2) providing more active catalysts than those pre-nitrided by ammonolysis.