For various reasons, low cost, easy fabrication, and so forth, dye-sensitized solar cells (DSSCs) have been consistently studied in many laboratories. To improve the DSSCs performance, using an aqueous solution of titanium tetrachloride (TiCl4) treatment is one of many processes. Before the treatment of TiCl4, nanoporous TiO2 nanotubes (TNTs) are fabricated through a secondary anodization process. TiCl4 treatment on TNTs film enhanced short-circuit current density (JSC) and aluminum oxide (Al2O3) posttreatment enhanced open-circuit voltage (VOC). As a result, Al2O3 posttreatment on TNTs film conversion efficiency of 8.65% is realized, which is 7% higher than TiCl4 treatment on TNTs film. In this work, we investigated that double dip-coating of TiCl4/Al2O3 treatment on TiO2 nanotubes film had an effect on enhancement of JSC and VOC due to improvement of electron transfer, increment of dye adsorption, and reduction of recombination rate of charge. Photoelectrode DSSCs with light-to-electric energy conversion efficiency were achieved under a simulated solar light irradiation of 100 mW·cm2 (AM 1.5).