We designed and fabricated multilayer quantum dots sensitized solar cells (QDSCs) with TiO2 NPs/CdSe0.3S0.7/CdSe/ZnSXSe1− X, X = S/S + Se = 0, 0.7, 0.8, 0.9, and 1 photoelectrodes to achieve optimum power conversion efficiency (PCE). In the corresponding structure, incoming light is absorbed by the CdSe0.3S0.7 and CdSe quantum dots (QDs), while the ZnSXSe1− X QDs act as an electron blocking layer or passivation layer, forming an energy barrier that restricts electron mobility from the light absorbers to the polysulfide electrolyte. The beneficial effect of the alloyed ZnSXSe1− X layer is the adjustability of its nanoparticle size/bandgap energy proportional to variations in the concentration of anionic precursors X, according to optical results. The PCE value of the reference cell with the TiO2 NPs/CdSe0.3S0.7/CdSe photoanode is 4.15 %. Following the coating of ZnSe, ZnS0.7Se0.3, ZnS0.8Se0.2, ZnS0.9Se0.1, and ZnS QDs via two successive ionic layer adsorption and reaction (SILAR) cycles (2Sc) on the CdSe0.3S0.7/CdSe co-sensitized photoelectrode increasing stability and improving the PCE value to 4.9 %, 5.40 %, 5.70, 5.25 %, and 5.05 %, respectively. Next, by modifying the thickness of the champion cell’s passivation layer, the QDSCs with TiO2 NPs/CdSe0.3S0.7/CdSe/ZnS0.8Se0.2 (3Sc) photoelectrode exhibit maximum photovoltaic performance parameters of short circuit current density (JSC) = 26.25 mA/cm2 , open circuit voltage (VOC) = 560 mV, fill factor (FF) = 0.42 % and PCE = 6.15 %. This improvement in performance is the result of decreased internal energy loss and recombination of charge carriers at the interface between the electrolyte and photoelectrode, which increases electron collection efficiency and electron injection efficiency in the visible region according to the external and internal quantum efficiency curves.