Pure Na 0.5 Sr 0.25 NbO 3 particles were successfully synthesized using the molten salt synthesis method in the SrCO 3 ?Nb 2 O 5 ?KCl?NaCl system, which could not be obtained in the SrCO 3 ?Nb 2 O 5 ?NaCl system. The result suggested that the fabrication process of Na 0.5 Sr 0.25 NbO 3 was different for the two systems. In the SrCO 3 ?Nb 2 O 5 ?NaCl system, NaSr 2 Nb 5 O 15 formed and then converted into Na 0.5 Sr 0.25 NbO 3 . In the SrCO 3 ?Nb 2 O 5 ?KCl?NaCl system, Na 0.5 Sr 0.25 NbO 3 could be obtained directly by the reaction between the intermediate KSN and NaCl. The effects of the NaCl salt content and heated temperature on the purity and size of particles were investigated. Pure Na 0.5 Sr 0.25 NbO 3 powder crystals with uniform particle size could be prepared at the heated temperature of 1,200°C and NaCl salt-to-oxide ratio of 2, which were ideal raw material for preparing Na 0.5 Sr 0.25 NbO 3 ceramics.