AbstractSpinel phase Zn2TiO4 powders were prepared by high‐temperature solution, which is a kind of molten salt (such as KCl melt). The effect of Zn2TiO4 synthesis was explored under different holding time, preparation temperature and the mass ratio of salt to raw material in KCl melt. Through experimental analysis, the synthesis temperature range of Zn2TiO4 phase in KCl molten salt system was from 800 to 1000 °C. Compared with the traditional solid‐state reaction, the stable temperature range of Zn2TiO4 phase in KCl molten salt system was wider. The HRTEM image analysis of calcined product was consistent with the XRD result. The TEM analysis showed that the average particle size of Zn2TiO4 powder was 200 nm. The crystallinity of Zn2TiO4 increased with increasing sintering time and Zn/Ti molar ratio. Compared with LiCl+KCl and LiCl melts, the crystallinity of Zn2TiO4 powder synthesized in KCl molten salt system was better. It is determined that the high‐temperature solution (KCl melt) can be successfully applied for large‐scale synthesis of spinel phase Zn2TiO4.