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Herein, we report a tetrahedral Zn(II) ion coordinated metal\u2212organic cage (\n                    <jats:bold>MOC<\/jats:bold>\n                    )\n                    <jats:bold>C3<\/jats:bold>\n                    constructed from a\n                    <jats:italic>\n                      C\n                      <jats:sub>3<\/jats:sub>\n                    <\/jats:italic>\n                    \u2010symmetric terpyridine ligand incorporating pyridinium units. In pure water under an O\n                    <jats:sub>2<\/jats:sub>\n                    atmosphere and without sacrificial agents,\n                    <jats:bold>C3<\/jats:bold>\n                    exhibits an H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    generation rate of 678.15 \u00b5mol L\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    . Moreover, the confined cavity of the\n                    <jats:bold>MOC<\/jats:bold>\n                    is proposed to help stabilize crucial intermediates (*OH from water oxidation and *OOH from oxygen reduction), thereby further promoting the catalytic performance. This work illustrates a ligand\u2010engineering strategy for photocatalyst design by employing functionalized ligands to construct\n                    <jats:bold>MOC<\/jats:bold>\n                    that primarily improve charge\u2010separation efficiency and create directional electron\u2010transfer channels within the cage framework, while the confined microenvironment secondarily stabilizes key reactive intermediates, thus offering a route toward advanced photocatalytic H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    generation.\n                  <\/jats:p>","DOI":"10.1002\/anie.202522655","type":"journal-article","created":{"date-parts":[[2026,1,27]],"date-time":"2026-01-27T13:11:32Z","timestamp":1769519492000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":7,"title":["Ligand\u2010Engineered Metal\u2013Organic Cages Boost Charge Separation for Efficient Photocatalytic Synthesis of Hydrogen Peroxide in Pure Water"],"prefix":"10.1002","volume":"65","author":[{"given":"Gang","family":"Chen","sequence":"first","affiliation":[{"name":"School of Civil Engineering C\/O Guangzhou Key Laboratory of Sensing Materials &amp; Devices Center For Advanced Analytical Science School of Chemistry and Chemical Engineering Guangzhou University  Guangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shutong","family":"Jiao","sequence":"additional","affiliation":[{"name":"Institute of Environmental Research at Greater Bay Area Key Laboratory for Water Quality and Conservation of the Pearl River Delta Ministry of Education Guangzhou University Guangzhou  China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qixia","family":"Bai","sequence":"additional","affiliation":[{"name":"College of Materials Science and Engineering Shanxi Normal University  Taiyuan 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