In order to overcome the defects of high electron-hole recombination rate and narrow absorption spectrum range of TiO2 nanotubes during photoelectric conversion, TiO2 nanotubes were synergistically modified by polyoxometalates H4SiW12O40 (SiW12) and CsPbI3 quantum dots. SiW12/TiO2 nanotube composite films were prepared by electrodeposition of SiW12 on TiO2 nanotubes. The CsPbI3 quantum dots were synthesized by high temperature thermal injection method, and then the CsPbI3 quantum dots were deposited on the composite films by chemical bath deposition method to obtain the SiW12/CsPbI3/TiO2 nanotube composite films. The effects of SiW12 deposition time and CsPbI3 deposition frequencies on the photoelectric properties of TiO2 nanotubes were investigated. The films were characterized by scanning electron microscopy (SEM), energy dispersive spectrometer (EDS), transmission electron microscope (TEM), X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), and ultraviolet visible spectrophotometer (UV-Vis). The photochemical properties of the films were tested by electrochemical workstation. The results show that the photoelectric conversion efficiency of TiO2 nanotubes deposited with polyoxometalates SiW12 and CsPbI3 quantum dots can be significantly improved by increasing the light absorption range and decreasing the charge transfer resistance up to 0. 52%. It shows that the synergistic effect of SiW12 and CsPbI3 can effectively inhibit the electron-hole recombination of TiO2 nanotubes, broaden the absorption spectrum and improve the photoelectric conversion efficiency of TiO2 nanotubes.