The overall objective of this research was the preparation of optical nanocomposite photoanodes through a simple method. The synthesized nanocomposite photoanodes were then used to improve the power conversion efficiency of dye-sensitized solar cells (DSSCs). Titanium dioxide (TiO2) nanofibers (NF) were prepared via electrospinning and calcination. Then, thin films were prepared with commercial TiO2 (NP) as a binder. Different concentrations of zinc oxide (ZnO) nanoparticles were used to impregnate TiO2 NP/NF. When the prepared nanostructures were used as photoanodes, the DSSCs based on NP/NF-ZnO film with an optimum concentration of ZnO (3.5 M) exhibited the highest short circuit current density (J(sc)) of 12.83 mA cm (2) and open circuit voltage (V-oc) of 0.764 V. The NP/NF-ZnO photoanode also exhibited a maximum power conversion efficiency (PCE) of 6.54%, which was higher by 26.5% than that of NP/NF (5.17%) with the same electrolyte.