At present, InP quantum dot-sensitized solar cells (QDSSCs) still show moderate power conversion efficiency (PCE), because of charge recombination on the surface defects. Herein, we report a method to reduce the surface defects of InP quantum dots by Ga-doped and ZnS shell coating, which improves the performance of InP QDSSCs. Simultaneous enhancement of photoluminescence (PL) and photo-electricity performance of Ga doped InP (Ga:InP) quantum dots (QDs), Ga:InP/ZnS core/shell QDs were achieved. The maximum PL quantum yield of Ga:InP QDs and Ga:InP/ZnS QDs reached 14.9% and 76%, respectively. The maximum PCE value of Ga:InP and Ga:InP/ZnS QDSSCs reached 3.0% and 4.5% under 1 sun illumination (AM 1.5 G, 100 mW/cm2), respectively. The J-V curve revealed that Ga doping and ZnS shell coating reduced the surface recombination and increased the cell efficiency and stability. These results provided a new approach to obtaining quantum dot materials with high luminescence properties or good solar cell performances.