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Here, a mesoporous NaY zeolite\u2010encapsulated atomically dispersed cobalt catalyst (Co@NaY\u2010M) is deliberately designed to be robust for single\u2010step, three\u2010component upgrading of biomass\u2010derived lactic acid, aldehydes, and anilines into 3,4\u2010unsubstituted quinolines via cascade dehydrogenation, annulation\u2013aromatization, and decarboxylation. Na\n                    <jats:sup>+<\/jats:sup>\n                    co\u2010dopant in zeolitic hexagonal prism adjacent to single\u2010atom Co in the supercage acts as an electron promoter to pull electrons from Co. The electron\u2010deficient Co improves formed intermediate adsorption\/activation, significantly declining energy barriers in cascade lactic\u2010acid\u2010to\u2010vinyl\u2010intermediate dehydrogenation, and 4\u2010substituted quinoline decarboxylation. Meanwhile, the presence of Na\n                    <jats:sup>+<\/jats:sup>\n                    strengthens interactions between Co and zeolitic carrier to improve the single\u2010atom stability. Co@NaY\u2010M has broad substrate scope for various 3,4\u2010unsubstituted quinolines with good compatibility to diverse functional groups in yields reaching 98% (&gt;80 examples) and can be scaled up (11.24\u00a0g). Importantly, the developed methodology enables direct synthesis of various clinical drugs. Life\u2010cycle\/techno\u2010economic investigations indicate that this protocol markedly lessens environmental footprints and is more price\u2010competitive compared to conventional quinoline synthesis methods. The precise modulation of neighboring zeolitic sites provides an effective avenue to directly access high\u2010value nitrogenous heterocycles from abundant renewables via oriented multiple reactions.\n                  <\/jats:p>","DOI":"10.1002\/anie.5647747","type":"journal-article","created":{"date-parts":[[2026,9,26]],"date-time":"2026-09-26T12:24:36Z","timestamp":1790425476000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Inter\u2010Cage Na\n                    <sup>+<\/sup>\n                    Enabling Single\u2010Atom Co for In Situ Delivery of Bio\u2010Based Vinyl Backbone to Access 3,4\u2010Unsubstituted Quinolines"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-6675-6279","authenticated-orcid":false,"given":"Feng","family":"Xu","sequence":"first","affiliation":[{"name":"State Key Laboratory of Green Pesticides State\u2010Local Joint Laboratory For Comprehensive Utilization of 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