By a solid-state process, well-crystallized BaTiO3 (BT) particles with their average grain size below 0.2 μm were obtained. Wet and dry mechanical pretreatment processes were combined to obtain fine particulate mixture comprising BaCO3 and TiO2 with the highest possible homogeneity without causing appreciable agglomeration. Degree of homogenization was quantitatively evaluated by different microscopic techniques, in an attempt to optimize nuclei-growth processes. Reaction processes were discussed on the basis of thermal analyses in conjunction with the particulate morphology. The granulometrical and crystallographical properties of the present particulate products are comparable with or even superior to commercially available high-valued products fabricated via a hydrothermal or sol-gel route.