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formation, and photoinduced halide segregation. Here, we report 4\u2010(3\u2010Carbamimidoylguanidino)benzoic acid hydrochloride (CGBA) as a precursor\u2010level regulator for Cs\/formamidinium (CsFA)\u2010based Br\u2010rich WBG perovskites. Through dynamic associations with lead\u2013halide species and organic cations, CGBA modifies the local precursor environment and alters the stage\u2010dependent film\u2010formation behavior during spin coating and annealing. This regulation moderates crystallization, promotes texture development, reduces trap\u2010mediated nonradiative recombination, and suppresses photoinduced halide segregation. Consequently, the optimized 1.78\u00a0eV single\u2010junction device achieves a power conversion efficiency (PCE) of 21.43% and a fill factor (FF) of 85.89%, placing it among the highest reported FF values for 1.75\u20131.79\u00a0eV single\u2010junction WBG perovskite solar cells. The strategy is also transferable across multiple compositions and conditions, yielding efficiencies of 27.32% (1.53\u00a0eV), 23.91% (1.68\u00a0eV), 18.75% (1.85\u00a0eV), and 26.08% (1.58\u00a0eV, antisolvent\u2010free). Unencapsulated target devices retain 93% of their initial efficiency after 4500\u00a0h in N\n                    <jats:sub>2<\/jats:sub>\n                    . When integrated into a monolithic all\u2010perovskite tandem, the CGBA\u2010optimized WBG subcell enables a laboratory\u2010measured PCE of 29.63%. This work establishes precursor\u2010level regulation as a transferable strategy for efficient and stable WBG perovskites and all\u2010perovskite tandems.\n                  <\/jats:p>","DOI":"10.1002\/adma.75165","type":"journal-article","created":{"date-parts":[[2026,9,27]],"date-time":"2026-09-27T07:14:38Z","timestamp":1790493278000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Precursor\u2010Level Molecular Coupling Enables High\u2010Fill\u2010Factor Wide\u2010Bandgap Perovskite Solar Cells and 29.63% All\u2010Perovskite Tandems"],"prefix":"10.1002","author":[{"given":"Kaixin","family":"Huang","sequence":"first","affiliation":[{"name":"School of Resources and Environmental Engineering University of South China  Hengyang China"},{"name":"Engineering and Research Center For Integrated New Energy Photovoltaics and Energy Storage Systems of Hunan Province and School of Electrical Engineering University of South 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