Fourier transform infrared analysis, nuclear magnetic resonance, and thermogravimetric analysis show that most of the solid product prepared from the reaction of Ti(OC4H9)(4) and excess (CH3CO)(2)O is a mixture of titanyl organic compounds. Nanocrystalline TiO2 particles, which include anatase TiO2, rutile TiO2, and a mixture of anatase and rutile, can be obtained from hydrolysis of the titanyl organic compounds under normal pressure at 60degreesC. The particle size, shape, and formation process of the crystals have been studied using X-ray diffraction and transmission electron microscopy. The specific-surface-area data for a rutile TiO2 sample and the powders obtained after calcination at different temperatures have been measured by the Brunauer-Emmett-Teller method.