SrAl2O4:Eu2+, Dy3+ phosphor was synthesized by chemical solution route to use as a dopant in TiO2 layer employed as a photoelectrode for down conversion of ultraviolet and near-ultraviolet to visible and near-infrared light in a dye-sensitized solar cell. Nano-crystalline structure of the SrAl2O4:Eu2+, Dy3+powder was confirmed by X-ray diffraction analysis and field emission scanning electron microscopy. Monitored at 520 nm, SrAl2O4:Eu2+, Dy3+ phosphor showed emission peaks at 460 to 610 nm due to 4f6 → 4f7 transitions of Eu2+ ions. For the study, SrAl2O4:Eu2+, Dy3+ phosphor-doped TiO2 layer was deposited on fluorine-doped tin oxide coated glass by electrostatic spray deposition. The short circuit current, open circuit voltage, fill factor, and conversion efficiency of the cells were measured. Experimental results revealed that the device efficiency for the SrAl2O4:Eu2+, Dy3+ phosphor-doped TiO2 layer increased to 7.20 %, whereas that of the pure-TiO2 photoelectrode was 4.13 %.