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Despite significant advances in the synthesis of \u03b1\u2010amino acids (\u03b1\u2010AAs) using CO\n                    <jats:sub>2<\/jats:sub>\n                    as carboxyl source, the direct \u03b1\u2010C(sp\n                    <jats:sup>3<\/jats:sup>\n                    )\u2212H carboxylation of primary amines, which are important organic chemical feedstocks, remains an attractive yet formidable challenge. Herein, we report the first visible\u2010light\u2010driven direct \u03b1\u2010C(sp\n                    <jats:sup>3<\/jats:sup>\n                    )\u2212H carboxylation of primary benzylamines with CO\n                    <jats:sub>2<\/jats:sub>\n                    , wherein CO\n                    <jats:sub>2<\/jats:sub>\n                    acts dually as a transient protecting group and as the carboxyl source. This strategy enables efficient synthesis of diverse \u03b1\u2010AAs under mild reaction conditions with a broad substrate scope and good functional group compatibility. Mechanistic studies indicate that an intermolecular hydrogen atom transfer (HAT) between the external HAT reagent and the carbamate intermediate, in situ\u2010generated from primary amine and CO\n                    <jats:sub>2<\/jats:sub>\n                    , is followed by reduction and carboxylation to furnish \u03b1\u2010AAs. Moreover, a complementary protocol for carboxylation of \u03b1\u2010C(sp\n                    <jats:sup>3<\/jats:sup>\n                    )\u2500H bonds in amides through an intramolecular 1,2\u2010HAT pathway is also developed, obviating the need for an external HAT reagent and further expanding the synthetic utility of this methodology. These advances represent a versatile and practical platform for the synthesis of \u03b1\u2010AAs from amine precursors using CO\n                    <jats:sub>2<\/jats:sub>\n                    .\n                  <\/jats:p>","DOI":"10.1002\/anie.202515737","type":"journal-article","created":{"date-parts":[[2025,9,25]],"date-time":"2025-09-25T10:07:38Z","timestamp":1758794858000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":23,"title":["Visible\u2010Light\u2010Driven \u03b1\u2010C(sp\n                    <sup>3<\/sup>\n                    )\u2212H Carboxylation of Primary Benzylamines with CO\n                    <sub>2<\/sub>\n                    to Access \u03b1\u2010Amino Acids"],"prefix":"10.1002","volume":"64","author":[{"given":"Xin\u2010Long","family":"Hu","sequence":"first","affiliation":[{"name":"Key Laboratory of Green Chemistry &amp; Technology of Ministry of Education College of Chemistry, Sichuan University  Chengdu 610064 P.R. 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