A novel perovskite intercalated nanomaterial HLaNb2O7/(Pt, TiO2) is fabricated by successive intercalated reaction of HLaNb2O7 with [Pt(NH3)4]Cl2 aqueous solution, n-C6H13NH2/C2H5OH organic solution and acidic TiO2 colloid solution, followed by ultraviolet light irradiation. The gallery height and the band gap energy of HLaNb2O7/(Pt, TiO2) is less than 0.6 nm and 3.14 eV, respectively. The photocatalytic activity of HLaNb2O7/TiO2 is superior to that of unsupported TiO2 and is enhanced by the co-incorporation of Pt. The photocatalytic hydrogen evolution based on HLaNb2O7/(Pt, TiO2) is 240 cm3 h−1 g−1 using methanol as a sacrificial agent under irradiation with wavelength more than 290 nm from a 100-W mercury lamp. High photocatalytic activity of HLaNb2O7/(Pt, TiO2) may be due to the host with rare earth La element and perovskite structure, the quantum size effect of intercalated semiconductor and the coupling effect between host and guest.