Recently,there has been renewed interest in interface engineering as a means to further push the perfor-mance of perovskite solar cells closer to the Schockly-Queisser limit.Herein,for the first time we employ a multi-functional 4-chlorobenzoic acid to produce a self-assembled monolayer on a perovskite surface.With this interlayer we observe passivation of perovskite surface defects and a significant suppression of non-radiative charge recombination.Furthermore,at the surface of the interlayer we observe,charge dipoles which tune the energy level alignment,enabling a larger energetic driving force for hole extrac-tion.The perovskite surface becomes more hydrophilic due to the presence of the interlayer.Consequently,we observe an improvement in open-circuit voltage from 1.08 to 1.16 V,a power conver-sion efficiency improvement from 18% to 21% and an improved stability under ambient conditions.Our work highlights the potential of SAMs to engineer the photo-electronic properties and stability of per-ovskite interfaces to achieve high-performance light harvesting devices.