Nickel ferrite (Ni 0.75 Fe 2.25 O 4 was synthesized by co-precipitation method in order to investigate its behavior under conditions of the reactor coolant system in pressurized light water nuclear power plants. Ammonia or potassium carbonate was used as a solution pH control agent, and aqueous ammonia or potassium carbonate solution or secondary distilled water was used as a co-precipitate washing agent. The effects of the pH control agent and the co-precipitate washing agent on the production yield on the basis of the Ni/Fe molar ratio and the particle characteristics of final products were investigated by XRD, SEM, EDX and XPS. The production yield was almost congruent with that of the initial aqueous mixture in case of using potassium carbonate as a pH control agent, while in case of using ammonia, it was quite changed. The difference seemed to be due to the effects of Ni 2+ ←NH 3 complexation in the aqueous solution and of the pH of co-precipitate washing agent.