TiO2 intercalated H4Nb6O17 has been synthesized by the reactions of H4Nb6O17 with a titanyl acylate complex followed by UV irradiation. The gallery height, specific surface area and Ti content of the sample synthesized by using titanyl acylate complex were larger than that using TiO2 sol solution. Furthermore, the photocatalytic activity of the TiO2 pillared H4Nb6O17 prepared using a titanyl acylate precursor was twice larger than that fabricated using a TiO2 sol solution.