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Here, we report the successful synthesis of Lewis acid\/base bimetallic nanocluster\n                    <jats:bold>\n                      Au\n                      <jats:sub>20<\/jats:sub>\n                      Mn\n                      <jats:sub>2<\/jats:sub>\n                    <\/jats:bold>\n                    and demonstrate its catalytic potential in visible\u2010light\u2010driven direct C(sp\n                    <jats:sup>2<\/jats:sup>\n                    )\u2013H arylation of aryl halides. The cluster comprises two Au\n                    <jats:sub>11<\/jats:sub>\n                    incomplete icosahedra fused into an Au\n                    <jats:sub>20<\/jats:sub>\n                    kernel, which features four uncoordinated gold atoms in a rhombic pattern and is protected by two bridged Mn(CO)\n                    <jats:sub>5<\/jats:sub>\n                    moieties. Experimental and computational studies disclose that the Mn sites function as electron donors, facilitating polarized Au(\u03b4\n                    <jats:sup>+<\/jats:sup>\n                    )\u2212Mn(\u03b4\n                    <jats:sup>\u2212<\/jats:sup>\n                    ) bonds with pronounced [Mn(CO)\n                    <jats:sub>5<\/jats:sub>\n                    ]\n                    <jats:sup>\u2212<\/jats:sup>\n                    \u2192Au\n                    <jats:sub>20<\/jats:sub>\n                    \u03c3 donation interactions. The Lewis acid\/base pair bestows\n                    <jats:bold>\n                      Au\n                      <jats:sub>20<\/jats:sub>\n                      Mn\n                      <jats:sub>2<\/jats:sub>\n                    <\/jats:bold>\n                    with exceptional photocatalytic performance in C(sp\n                    <jats:sup>2<\/jats:sup>\n                    )\u2013H arylation of various substituted (hetero)aryl bromides and chlorides with electron\u2010rich\u2010to\u2010deficient arenes under mild conditions. This protocol boasts high functional group tolerance, supports gram\u2010scale synthesis, and is applicable to both the late\u2010stage functionalization of complex molecules and the targeted synthesis of bioactive products. Mechanism analyses uncover that the collaboration between the gold\u2010involved single electron transfer activation of aryl halides and Mn \u03c0\u2010base activation of arenes accounts for the remarkable efficiency of this system.\n                  <\/jats:p>","DOI":"10.1002\/anie.7471740","type":"journal-article","created":{"date-parts":[[2026,7,10]],"date-time":"2026-07-10T15:20:57Z","timestamp":1783696857000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Lewis Acid\/Base Au\u2013Mn Pairs in Metal Nanoclusters for Enhanced Photocatalytic C(sp\n                    <sup>2<\/sup>\n                    )\u2013H Arylation"],"prefix":"10.1002","volume":"65","author":[{"given":"De\u2010Bo","family":"Hao","sequence":"first","affiliation":[{"name":"State Key Laboratory of Bioactive Molecules and Druggability Assessment Guangdong Basic Research Center of Excellence for Natural Bioactive Molecules and Discovery of Innovative Drugs College of Chemistry and Materials Science and Guangdong Provincial Key Laboratory of Supramolecular Coordination Chemistry Jinan University  Guangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lin\u2010Mei","family":"Zhang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Bioactive Molecules and Druggability Assessment Guangdong Basic Research Center of Excellence for Natural Bioactive Molecules and Discovery of Innovative Drugs College of Chemistry and Materials Science and Guangdong Provincial Key Laboratory of Supramolecular Coordination Chemistry Jinan University  Guangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Si\u2010Rui","family":"Shen","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Bioactive Molecules and Druggability Assessment Guangdong Basic Research Center of Excellence for Natural Bioactive Molecules and Discovery of Innovative Drugs College of Chemistry and Materials Science and Guangdong Provincial Key Laboratory of Supramolecular Coordination Chemistry Jinan University  Guangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lan\u2010Fang","family":"Liang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Bioactive Molecules and Druggability Assessment Guangdong Basic Research Center of Excellence for Natural Bioactive Molecules and Discovery of Innovative Drugs College of Chemistry and Materials Science and Guangdong Provincial Key Laboratory of Supramolecular Coordination Chemistry Jinan University  Guangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xu\u2010Hang","family":"Zhong","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Bioactive Molecules and Druggability Assessment Guangdong Basic Research Center of Excellence for Natural Bioactive Molecules and Discovery of Innovative Drugs College of Chemistry and Materials 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