We describe a flexible and competent solution for fabrication of non-prefabricated nanocrystal mesoporous TiO2-based photoanodes whose thicknesses are tunable from several hundreds of nanometers up to 12.4 microm. The combination of rapid thermal process and layer-by-layer spin-coating is successfully used to manipulate the structure and morphology of non-prefabricated nanocrystal mesoporous TiO2 films. The photovoltaic performances of mesoporous TiO2-based dye-sensitized solar cells depended on the thickness and the annealing temperature of mesoporous photoanodes. We systematically investigated and noted that the non-prefabricated nanocrystal mesoporous TiO2 films approximately 6.3 microm thick annealed at 500 degrees C displayed better features in the short-circuit current density and overall conversion efficiency of mesoporous TiO2-based dye-sensitized solar cells.