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Herein, we propose an interface ionic engineering strategy to address this issue. Specifically, a multifunctional N\u2010(4\u2010Cyanophenyl)guanidine hydrochloride (NCGCl) salt with multiple hydrophilic functional groups is employed to modify the SAM layer to overcome the perovskite solution spreading problem. We demonstrate that the nitrile and guanidinium groups in NCGCl strongly interact with perovskite components, facilitating heterogeneous nucleation and defect passivation. Moreover, the\n                    <jats:italic>\u03c0\u2013\u03c0<\/jats:italic>\n                    * stacking between the benzene rings in NCGCl and SAMs further strengthens the substrate\u2010perovskite interface bridging. Consequently, the antisolvent\u2010free processed PSCs on rigid and flexible substrates demonstrate champion PCEs of 26.89% (certified 26.64%) and 25.29%, respectively. We also fabricate 5\u00a0cm\u00a0\u00d7\u00a05\u00a0cm flexible mini\u2010modules, showing an impressive PCE of 22.28%, along with outstanding mechanical bending stability.\n                  <\/jats:p>","DOI":"10.1002\/adma.73358","type":"journal-article","created":{"date-parts":[[2026,5,12]],"date-time":"2026-05-12T13:07:26Z","timestamp":1778591246000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Enhancing Heterogeneous Nucleation on Buried Interface for Efficient Antisolvent\u2010Free Inverted Flexible Perovskite Photovoltaics"],"prefix":"10.1002","volume":"38","author":[{"ORCID":"https:\/\/orcid.org\/0009-0009-2052-3937","authenticated-orcid":false,"given":"Fei","family":"Wang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Advanced Technology For Materials Synthesis and Processing Wuhan University of Technology  Wuhan P. R. China"},{"name":"Foshan Xianhu Laboratory  Foshan P. R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2422-4650","authenticated-orcid":false,"given":"Shaohang","family":"Wu","sequence":"additional","affiliation":[{"name":"Institute of New Energy Technology Jinan University  Guangzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7623-686X","authenticated-orcid":false,"given":"Sai","family":"Bai","sequence":"additional","affiliation":[{"name":"Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of China  Chengdu P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8635-9262","authenticated-orcid":false,"given":"Fuzhi","family":"Huang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Advanced Technology For Materials Synthesis and Processing Wuhan University of Technology  Wuhan P. R. 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