The purpose of this work is to introduce an improved MSS process so that single-phase CaZrO3 powder could be synthesized at an even lower temperature by heating a mixture of CaCl2, Na2CO3, and ZrO2 powders. The effects of processing factors (e.g., heating temperature and time) on the formation of the CaZrO3 phase have been investigated, and the synthesis mechanisms have been discussed based on the experimental results and thermodynamic analysis.