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Abstract Self‐assembled monolayers (SAMs) employed in inverted perovskite solar cells (PSCs) have achieved groundbreaking progress in device efficiency and stability for both single‐junction and tandem configurations, owing to their distinctive and versatile ability to manipulate chemical and physical interface properties. In this regard, we present a comprehensive review of recent research advancements concerning SAMs in inverted perovskite single‐junction and tandem solar cells, where the prevailing challenges and future development prospects in the applications of SAMs are emphasized. We thoroughly examine the mechanistic roles of diverse SAMs in energy‐level regulation, interface modification, defect passivation, and charge transportation. This is achieved by understanding how interfacial molecular interactions can be finely tuned to mitigate charge recombination losses in inverted PSCs. Through this comprehensive review, we aim to provide valuable insights and references for further investigation and utilization of SAMs in inverted perovskite single‐junction and tandem solar cells.