When titanium tetrachloride and acetic anhydride were mixed, an acute reaction occurred immediately. The products, titanyl acetate chloride organic compounds, were studied with FTIR and TGA. The results indicated that the), were composed of two dimmers [(CH3CO2TiOCl)(2) and (CH3CO2TiCl2)(2)O] in which a Ti atom combined with acetate in the way of coordinative bonding. In those dimmers, there are frameworks of Ti-O-Ti chemical bridges that are favorable units for forming nanosized crystalline titania. At low temperature (60 degrees C) and normal pressure, the titanyl acetate chloride organic compounds can hydrolyze to form nanosized crystalline anatase titania globate particles, 5-7 nm in size, which were approved by XRD (x-ray diffraction), TEM (transmission electron microscope), and LS (laser scattering). And more, the experiments of photocatalytic degradation of the dye rohdamine B revealed the nanosized crystalline anatase titania powders prepared with titanium tetrachloride and acetic anhydride as materials have a good photocatalytic activity.