TiCl4 treatment was used to chemically agglomerate TiO2 primary nano-particles to form a nanostructured powder in size of submicrometer. Nanocrystalline TiO2 coatings were fabricated by vacuum cold spraying at room temperature using the powder and were employed to assemble dye-sensitized solar cells. TiO2 coating of 10-20μm in thickness was deposited successfully on both F-doped tin oxide (FTO) conducting glass and plastic conducting substrate. The assembled solar cell with an FTO conducting glass yielded a short-circuit current density of 9.7 mA/cm2 and an energy conversion efficiency of 3.3%. Using the plastic substrate, the cell efficiency was 1.9%. These results suggest that TiCl4-treated nanocrystalline TiO2 agglomerates can be used to deposit TiO2 coating by vacuum cold spraying at low temperature for flexible dye-sensitized solar cells.