Calcium zirconate (CaZrO3) powder was synthesized using calcium chloride (CaCl2), sodium carbonate (Na2CO3), and zirconia (ZrO2) powders. On heating, CaCl2 reacted with Na2CO3 to form NaCl and CaCO3. NaCl–Na2CO3 molten salts provided a liquid reaction medium for the formation of CaZrO3 from in situ-formed CaCO3 (or CaO) and ZrO2. CaZrO3 started to form at about 700°C, increasing in amount with increasing temperature and reaction time, with a concomitant decrease in CaCO3 (or CaO) and ZrO2 contents. After washing with hot-distilled water, the samples heated for 5 h at 1050°C were single-phase CaZrO3 with 0.5–1.0 μm grain size.