BaTiO3 powders were prepared through mechanical activation chemistry and analyzed by Rietveld refinement with X-ray diffraction data. Raw BaCO3 and TiO2 powders were dry milled for 5 and 20 h and then calcinated for 2 and 4 h at 800 °C. The milling process was found to have broken up the BaCO3 and TiO2 crystals into smaller crystals and formed only small amounts (<1.5 wt%) of BaTiO3. Subsequence calcinations for 2 and 4 h at 800 °C successfully produced large amounts (>97.7 wt%) of BaTiO3 crystals. The calcination process also generated microstrains and crystallite-size anisotropy in BaTiO3. An increase in the calcination time from 2 to 4 h increased the BaTiO3 weight percentage and the crystallite-shape anisotropy, but decreased the tetragonal distortion anisotropic microstrains in BaTiO3 crystals.