In most current state-of-the-art perovskite solar cells (PSCs), high-temperature (approximate to 500 degrees C)-sintered metal oxides are employed as electron-transporting layers (ETLs). To lower the device processing temperature, the development of low-temperature-processable ETL materials (such as solution-processed ZnO) has received growing attention. However, thus far, the use of solutionprocessed ZnO is limited because the reverse decomposition reaction that occurs at ZnO/perovskite interfaces significantly degrades the charge collection and stability of PSCs. In this work, the reverse decomposition reaction is successfully retarded by sulfur passivation of solution-processed ZnO. The sulfur passivation of ZnO by a simple chemical means, efficiently reduces the oxygen-deficient defects and surface oxygen-containing groups, thus effectively preventing reverse decomposition reactions during and after formation of the perovskite active layers. Using the low-temperature-processed sulfurpassivated ZnO (ZnO-S), perovskite layers with higher crystallinity and larger grain size are obtained, while the charge extraction at the ZnO/perovskite interface is significantly improved. As a result, the ZnO-S-based PSCs achieve substantially improved power-conversion-efficiency (PCE) (19.65%) and long-term air-storage stability (90% retention after 40 d) compared with pristine ZnO-based PSCs (16.51% and 1% retention after 40 d). Notably, the PCE achieved is the highest recorded (19.65%) for low-temperature ZnObased PSCs.