Because of unique dielectric, piezoelectric, thermoelectric, optical and ferroelectric properties of titanates of alkaline earth metals, they have become an object of many scientific research. This article is concerned with mechanochemical synthesis of calcium titanate as an alternative technique to hydrothermal, sol–gel, thermal methods. The aim of this study was to verify the mechanochemical conditions of CaTiO3 formation with the use of three calcium oxide precursors—CaO, CaCO3 and Ca(OH)2. The differences in processes of calcium titanate synthesis are presented.