Nanocrystalline titania films codoped with aluminum and boron were prepared by cathodic vacuum arc deposition. In the process, titanium alloy target was used under an O2/Ar atmosphere, and sensitization of films were carried out by natural dye-sensitized complex in anhydrous ethanol. The structure, surface morphology and UV-vis spectra of titania films codoped were measured by X-ray diffraction analysis, scanning electron microscopy and ultraviolet-visible spectrometer. Theas-deposited films are found to be amorphous. The films annealed were examinedto be of anatase structure with orientation along the (101) planes, the averagecrystal size is in the range between 41 and 45 nm. SEM results show that thereare some pores in the codoped titania films, the optical properties of the dye-sensitized films were also measured which reveals that the spectral responses of films shift to the visible region. Under simulated sunlight illumination, the overall energy conversion efficiency of dye-sensitized nanocrystalline solar cell is 0.9%.