We used the SCAPS-1D simulation tool to maximize the performance of lead sulfide (PbS) solar cells. A PbS solar cell was first modeled and then experimentally verified from past research. The ZnO electron-transport layer (ETL) was then replaced with ZnO:Al ETL material. Additionally, the fluorine-doped tin oxide work function, PbS-TBAI, ZnO:Al layer thicknesses, ZnO:Al/PbS-TBAI, PbS-TBAI/PbS-EDT defect density, PbS-TBAI defect density, ZnO:Al, and PbS-TBAI doping concentration were optimized. Results showed a greater alignment of the absorber-layer valence band with the HOMO and LUMO of ZnO:Al than that of ZnO ETL. The PbS solar cell exhibited the greatest efficiency at the optimum values of 0.4 µm, 0.04 µm, 1019 cm–3, 4.0 eV, 1017 cm–3, 1014 cm–2, 1018 cm–2, and 3.8 eV for absorber thickness, ETL thickness, ETL doping concentration, work function of front contact, PbS-TBAI doping concentration, and electron affinity of ZnO:Al, respectively. The PbS solar cell also performed best at interface defect densities of 1014 and 1018 cm–2 for ZnO:Al/PbS-TBAI and PbS-TBAI/PbS-EDT, respectively. The PCE of ZnO:Al ETL-based device also increased from 15.036% before optimization to 19.169% after. The optimized result was found to be affected by temperature. The PbS-optimized device with inorganic hole-transport layers (HTLs) demonstrated higher performance than the device with organic HTL. This finding was attributed to the low hole mobility in the organic HTL than those of inorganic ones. Therefore, the ZnO:Al ETL-based device was more efficient than the ordinary ZnO ETL-based device.