In this article, mechanochemical synthesis of barium titanate from different raw materials was studied. The prepared nanodispersed powders were investigated by means of XRD, DTA-TG, DSC, FTIR, Raman, UV–VIS, ESR spectroscopy, and low-temperature adsorption of nitrogen. Barium titanate possessing high specific surface area was produced directly during dry milling from the mixtures of barium oxides and titanium dioxide low-temperature forms (amorphous and anatase).