Nanocomposites of Titania-ZnO with molar ratios 2:1(TZ-S1) and 3:1(TZ-S2) were synthesized by employing a modified sol-gel method. The prepared nanocomposites were characterized employing X-ray diffraction (XRD), scanning electron microscopy (SEM), energy dispersive X-ray analysis (EDAX), UV, and BET analysis. The crystallinity and morphology of the nanostructures were compared for varying molar concentrations. The nanostructures thus synthesized were employed as photo-anode semiconductor materials in the fabrication of Dye- Sensitized Solar Cells (DSSC). The DSSC developed with the photo-anode of Titania-ZnO with a molar ratio of 3:1 exhibited better photovoltaic performance with an efficiency of 0.77% and a current density of 3.89 mA/cm2 than the device with nanocomposites of TiO2- ZnO with molar ratio 2:1.