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Abstract: Herein, this study reports high‐efficiency, low‐temperature ZnO based planar perovskite solar cells (PSCs) with state‐of‐the‐art performance. They are achieved via a strategy that combines dual‐functional self‐assembled monolayer (SAM) modification of ZnO electron accepting layers (EALs) with sequential deposition of perovskite active layers. The SAMs, constructed from newly synthesized molecules with high dipole moments, act both as excellent surface wetting control layers and as electric dipole layers for ZnO‐EALs. The insertion of SAMs improves the quality of PbI2 layers and final perovskite layers during sequential deposition, while charge extraction is enhanced via electric dipole effects. Leveraged by SAM modification, our low‐temperature ZnO based PSCs achieve an unprecedentedly high power conversion efficiency of 18.82% with a VOC of 1.13 V, a JSC of 21.72 mA cm−2, and a FF of 0.76. The strategy used in this study can be further developed to produce additional performance enhancements or fabrication temperature reductions. [ABSTRACT FROM AUTHOR]