Ultrafine BaTiO3 prepared by a decomposition of an organometallic crystal with unity of Ba/Ti ratio (sol-crystal method) has been characterized. While the as-prepared product resulting from the decomposition of the organometallic crystal at room temperature was BaTiO3 with pseudo-cubic structure, the well-crystallized tetragonal polymorph was obtained by firing the as-prepared product above 1000°C. Residual organic compounds, CO2-3 and OH- ions in the samples prevent the grain growth and tetragonal distortion of BaTiO3. We obtained quite higher room temperature permittivity (3700) at 1 kHz for the sample fired at 1200°C than that (630) prepared by conventional solid-state reaction starting from BaCO3 and TiO2. Such a high value was probably due to the accomplishment of homogeneous cation stoichiometry, which was achieved by this preparation method via the organometallic crystal with stoichiometric Ba/Ti ratio.