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Here, we report an electrostatic potential (ESP)\u2010guided approach to construct nitrogen\u2010containing polycyclic aromatic self\u2010assembled monolayers (SAMs) that address this challenge. By integrating a rigid, planar perylenocarbazole (PCz) core with extended \u03c0\u2010conjugation, alkyl chain optimization, and bromination, we designed two novel SAMs, 4PCzBr and 6PCzBr, with precisely tailored ESP distributions. Compared to conventional carbazole\u2010based SAMs, these designs substantially elevate the average ESP, strengthen intermolecular \u03c0\u2013\u03c0 interactions, and promote dense, ordered monolayer formation on ITO, thereby enhancing work function alignment and hole extraction. Interestingly, the elevated ESP of 6PCzBr strengthens electrostatic interactions with the donor PM6, driving preferential donor crystallization at the buried interface and establishing an ideal vertical phase separation for efficient charge transport. Leveraging this synergy, 6PCzBr\u2010based OSCs deliver an outstanding efficiency of 20.16%, while inverted PSCs achieve a remarkable efficiency of 26.20% with decent operation stability. This work establishes ESP\u2010engineered polycyclic aromatic SAMs as a versatile interfacial platform bridging organic and perovskite photovoltaics, offering a broadly applicable molecular design paradigm for high\u2010efficiency and stable solar cells.<\/jats:p>","DOI":"10.1002\/anie.4031162","type":"journal-article","created":{"date-parts":[[2026,7,7]],"date-time":"2026-07-07T14:06:13Z","timestamp":1783433173000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Perylenocarbazole\u2010Based Polycyclic Aromatic Self\u2010Assembled Monolayers with Tailored Electrostatic Potentials for High\u2010Performance Organic and Perovskite Solar Cells"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0009-0003-3706-2483","authenticated-orcid":false,"given":"Xing","family":"Chen","sequence":"first","affiliation":[{"name":"Key Laboratory of Fluorine and Silicon for Energy Materials and Chemistry of 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