Bimodal mesoporous titania powders with high photocatalytic activity were prepared by hydrolysis of titanium tetraisopropoxide in the presence of HNO 3 or NH 4OH under ultrasonic irradiation. The powders were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), BET surface areas, and X-ray photoelectron spectroscopy (XPS). Photocatalytic activity was evaluated by the photocatalytic oxidation of acetone in air. The effects of catalysts added during hydrolysis on the microstructure and photocatalytic activity of the TiO 2 powders were investigated. The results showed that HNO 3 enhanced the growth of brookite, while NH 4OH not only retarded phase transformation of the TiO 2 powders from amorphous to anatase and anatase to rutile but also suppressed the growth of brookite. All TiO 2 powders calcined from 400 to 600 °C showed bimodal pore-size distributions in the mesoporous region: one was intraaggregated pores with maximum pore diameters of ca. 4–9 nm and the other interaggregated ones with maximum pore diameters of ca. 35–50 nm. At 700 °C, the pore-size distributions of all samples exhibited monomodal distribution of the interaggregated pores due to the collapse of the intraaggregated pores. The photocatalytic activity of the TiO 2 powders prepared by this method and calcined at 400 °C exceeded that of Degussa P-25 when the molar ratio of HNO 3 or NH 4OH to H 2O was less than 0.05.