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Herein, we report a bifunctional MOF, Hf\u2010VIO\u2010DBP, that integrates porphyrinic photosensitizers (DBP) and viologen electron mediators (VIO\n                    <jats:sup>2+<\/jats:sup>\n                    ) within a single framework to establish a dual\u2010channel photoactive platform. The close spatial proximity of these two functional units enables efficient intra\u2010framework electron transfer while preserving the energy transfer capability of the porphyrinic photosensitizers. Upon 630 nm irradiation, excited DBP transfers electrons to VIO\n                    <jats:sup>2+<\/jats:sup>\n                    to generate viologen radical species, which mediate O\n                    <jats:sub>2<\/jats:sub>\n                    reduction to generate type I ROS, including superoxide, hydrogen peroxide, and hydroxyl radicals. The resulting DBP radical cation is reduced by endogenous biomolecules such as 1,4\u2010dihydronicotinamide adenine dinucleotide, thereby regenerating DBP and sustaining the photoredox cycle. Concurrently, energy transfer from excited DBP to O\n                    <jats:sub>2<\/jats:sub>\n                    produces singlet oxygen through a type II pathway. Compared with the viologen\u2010free MOF analogue, Hf\u2010VIO\u2010DBP markedly enhances type I ROS generation while retaining efficient type II ROS production, resulting in substantially improved overall ROS yields and phototoxicity. Therefore, Hf\u2010VIO\u2010DBP achieves potent PDT efficacy in CT26 and MC38 murine colon cancer models.\n                  <\/jats:p>","DOI":"10.1002\/anie.7283158","type":"journal-article","created":{"date-parts":[[2026,10,13]],"date-time":"2026-10-13T05:48:58Z","timestamp":1791870538000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Bifunctional Metal\u2013Organic Frameworks Integrate Energy\u2010 and Electron\u2010Transfer Pathways for Enhanced Photodynamic Therapy"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-8240-2190","authenticated-orcid":false,"given":"Zhibei","family":"Zhou","sequence":"first","affiliation":[{"name":"Department of Chemistry The University of Chicago  Chicago Illinois USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuxuan","family":"Xiong","sequence":"additional","affiliation":[{"name":"Department of Chemistry The University of Chicago  Chicago Illinois USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8774-3733","authenticated-orcid":false,"given":"Daqian","family":"Bian","sequence":"additional","affiliation":[{"name":"Department of Chemistry The University of Chicago  Chicago Illinois USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7035-7759","authenticated-orcid":false,"given":"Wenbin","family":"Lin","sequence":"additional","affiliation":[{"name":"Department of Chemistry Westlake University  Hangzhou Zhejiang China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,10,12]]},"reference":[{"key":"e_1_2_8_2_1","doi-asserted-by":"crossref","first-page":"673","DOI":"10.1021\/cr300014x","article-title":"Introduction to Metal\u2212Organic Frameworks","volume":"112","author":"Zhou H.\u2010C.","year":"2012","journal-title":"Chemical Reviews"},{"key":"e_1_2_8_3_1","doi-asserted-by":"crossref","first-page":"3","DOI":"10.1016\/j.micromeso.2004.03.034","article-title":"Metal\u2013Organic Frameworks: A New Class of Porous Materials","volume":"73","author":"Rowsell J. 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