A new method has been developed for surface treatment of TiO2 photoanodes with LiI/NaI to enhance the photocurrent and, subsequently, the performance efficiency of the fabricated dye-sensitized solar cells (DSSCs). Three different concentrations (0.1, 0.25, and 0.5 mmol%) of LiI and NaI solutions were used to investigate the effect of this surface treatment on the device performance of DSSCs. A positive shift in the energy level of TiO2 has been experienced by surface treated devices, which is predominantly supported by the decrease in VOC. Furthermore, the introduction of LiI/NaI onto the TiO2 surface resulted in a reduction in the crystallite size, indicating an increase in the surface area which helps in more dye adsorption leading to higher JSC values of the devices. Besides, modification of the conduction band energy level, it also allows a fast electron injection process by shifting the density of states. Thus, this approach offers a simple but efficient route to enhance the photocurrent and efficiency of DSSCs.