The mineral was discovered in the Ural Mountains of Russia by Gustav Rose in 1839 and named after Russian mineralogist Lev Perovski (1792–1856).
Victor Goldschmidt described the perovskite structure in 1926 using tolerance factors — stability between 0.75 and 1.0 — and Helen Dick Megaw refined it in 1945 from barium titanate X-ray data.
CaTiO₃ crystallizes with lattice constants a = 5.39 Å, b = 5.45 Å, c = 7.65 Å and high refractive indices of 2.30 to 2.38.