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In this study, we introduce electrostatically buffered radical coupling (EBRC) as an alternative electronic\u2010coupling mode for activating organic sublattices. By inserting an electrostatic buffering medium between neighboring organic radicals, EBRC alleviates the intrinsic limitation of direct radical \u03c0\u2010stacking, where strong Coulombic repulsion within partially filled radical bands promotes Mott\u2013Hubbard\u2010type localization. Using photochromic viologen\u2010based hybrid perovskites as model systems, we directly compare EBRC with conventional compact radical \u03c0\u2010stacking. Counterintuitively, despite the larger intermolecular separation and reduced orbital overlap, the EBRC system exhibits an approximately 100\u2010fold enhancement in conductivity and photocurrent, whereas the compact radical \u03c0\u2010stacked counterpart shows only negligible improvement. The EBRC system further increases carrier mobility by approximately 70\u2010fold, facilitates efficient organic\u2013inorganic electron transport, and enables light\u2010induced reversible reconstruction of the band\u2010edge electronic structure. These findings establish electrostatic buffering as a complementary design principle for engineering intermolecular electronic coupling beyond the conventional orbital\u2010overlap paradigm, providing a general framework for activating electronically functional organic sublattices in perovskites and related radical semiconductors.<\/jats:p>","DOI":"10.1002\/anie.8462867","type":"journal-article","created":{"date-parts":[[2026,10,24]],"date-time":"2026-10-24T07:11:13Z","timestamp":1792825873000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Activating Electronic Functionality of Organic Sublattices in Hybrid Perovskites Through Electrostatically Buffered Radical Coupling"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0001-1881-5895","authenticated-orcid":false,"given":"De\u2010Lin","family":"Hu","sequence":"first","affiliation":[{"name":"State Key Laboratory of Structural Chemistry Fujian 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