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Perovskite solar cells (PSCs) suffer from a quick efficiency drop after fabrication, partly due to surface defects, and efficiency can be further enhanced with the passivation of surface defects. Herein, surface passivation is reviewed as a method to improve both the stability and efficiency of PSCs, with an emphasis on the chemical mechanism of surface passivation. Various molecules are utilized as surface passivants, such as halides, Lewis acids and bases, amines (some result in low-dimensional perovskite), and polymers. Multifunctional molecules are a promising group of passivants, as they are capable of passivating multiple defects with various functional groups. This review categorizes these passivants, in addition to considering the potential and limitations of each type of passivant. Additionally, surface passivants for Sn-based PSCs are discussed since this group of PSCs has poor photovoltaic performance compared to their lead-based counterpart due to their severe surface defects. Lastly, future perspectives on the usage of surface passivation as a method to improve the photovoltaic performance of PSCs are addressed to provide a direction for upcoming research and practical applications.