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Here, we report an interfacial engineering strategy that goes beyond conventional SAM modification by introducing a thiophen\u20103\u2010ylmethanamine hydrochloride (3\u2010TMA) molecular layer between the SAM and perovskite photo\u2010active layer. The aromatic thiophene units establish strong\n                    <jats:italic>\u03c0<\/jats:italic>\n                    \u2011\n                    <jats:italic>\u03c0<\/jats:italic>\n                    stacking interactions with the underlying SAM, forming a solvent\u2010resistant interlayer that stabilizes the anchored SAM structure during solution processing. Meanwhile, hydrogen\u2010bonding interactions between 3\u2010TMA and the perovskite precursors effectively decelerate crystallization, promoting uniform nucleation and high\u2010quality WBG perovskite films. The resulting interface exhibits improved energy\u2010level alignment and reduced interfacial stress, facilitating efficient charge transport and enhanced device stability. Consequently, single\u2010junction WBG perovskite devices with bandgaps of 1.67 and 1.84\u00a0eV achieve champion power conversion efficiencies (PCEs) of 23.17% and 19.61%, respectively. When integrated into monolithic perovskite\u2012silicon TSCs, the strategy enables PCEs of 33.21% (certified 32.13%) for rigid tandems and 31.03% (certified 30.34%) for flexible tandems. Encapsulated devices retain 92.3% of their initial performance after 1000 h of continuous 1 sun illumination at room temperature.\n                  <\/jats:p>","DOI":"10.1002\/anie.1676645","type":"journal-article","created":{"date-parts":[[2026,7,22]],"date-time":"2026-07-22T05:21:22Z","timestamp":1784697682000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Beyond Self\u2010Assembled Molecules: Hydrogen\u2010Bonding\u2010Regulated Crystallization of Wide\u2010Bandgap Perovskite for High\u2010Performance Perovskite\u2010Silicon Tandem Photovoltaics"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0009-0000-2442-4076","authenticated-orcid":false,"given":"Fei","family":"Wang","sequence":"first","affiliation":[{"name":"Research Center for New Energy Technology (RCNET) National Key Laboratory of Materials for Integrated Circuits Shanghai Institute of Microsystem and Information Technology (SIMIT) Chinese Academy of Sciences (CAS)  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Taomiao","family":"Wang","sequence":"additional","affiliation":[{"name":"Hoffmann Institute of Advanced Materials Shenzhen Polytechnic University  Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuhui","family":"Ji","sequence":"additional","affiliation":[{"name":"Research Center for New Energy Technology (RCNET) National Key Laboratory of Materials for Integrated Circuits Shanghai Institute of Microsystem and Information Technology (SIMIT) Chinese Academy of Sciences (CAS)  Shanghai China"},{"name":"School of New Energy and Materials Southwest Petroleum University  Chengdu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Junjun","family":"Li","sequence":"additional","affiliation":[{"name":"Research Center for New Energy Technology (RCNET) National Key Laboratory of Materials for Integrated Circuits Shanghai Institute of Microsystem and Information Technology (SIMIT) Chinese Academy of Sciences (CAS)  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jianliang","family":"Wang","sequence":"additional","affiliation":[{"name":"Laboratory of Environmental Sciences and Technology Xinjiang Technical Institute of Physics &amp; 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