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Notably, their electrical performance is closely related to the packing and ligand oxidation state within the framework, which has rarely been explored. Typical divalent metal nodes favor saturated intralayer square\u2010planar coordination to ligands in a single oxidation state, thereby predetermining the framework topology. Here, we report a packing and topology control strategy, achieved by tuning the ligand oxidation state and grounded in lanthanides (e.g., Gd) versatile coordination chemistry. Diffuse reflectance spectroscopy and single\u2010crystal transport measurements reveal that, at low temperature, coordination of Gd\n                    <jats:sup>3+<\/jats:sup>\n                    with 2,3,6,7,10,11\u2010hexahydroxytriphenylene (HHTP) in a lower mixed oxidation state (\u22124 and \u22125) yields a more ordered porous packing (Gd\n                    <jats:sub>1.5<\/jats:sub>\n                    HHTP) with superior electronic transport performance. In contrast, at elevated temperature, the ligand adopts a higher oxidation state (\u22123), and coordination with Gd\n                    <jats:sup>3+<\/jats:sup>\n                    yields a densely packed structure with local coordination disorder (GdHHTP), resulting in a markedly reduced electrical conductivity. This study demonstrates ligand\u2010oxidation\u2010state tuning provides an effective strategy for the precise control of structural order and charge transport in c\u2010MOFs, laying a theoretical foundation for the rational design of materials with tunable electronic properties.\n                  <\/jats:p>","DOI":"10.1002\/anie.202522424","type":"journal-article","created":{"date-parts":[[2025,12,8]],"date-time":"2025-12-08T14:27:15Z","timestamp":1765204035000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["Packing Order Control in Conductive Metal\u2013Organic Frameworks by Tuning Ligand Oxidation State"],"prefix":"10.1002","volume":"65","author":[{"given":"Yunlong","family":"Fan","sequence":"first","affiliation":[{"name":"Key Laboratory of Artificial Structure and Quantum Control Ministry of Education School of Physics and Astronomy Shanghai Jiao Tong University  Shanghai 200240 P.R. China"},{"name":"National Key Laboratory of Advanced Micro and Nano Manufacture Technology Key Laboratory of Polymer Chemistry and Physics of Ministry of Education School of Materials Science and Engineering Peking University  Beijing 100871 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bin","family":"Jiang","sequence":"additional","affiliation":[{"name":"National Key Laboratory of Advanced Micro and Nano Manufacture Technology Key Laboratory of Polymer Chemistry and Physics of Ministry of Education School of Materials Science and Engineering Peking University  Beijing 100871 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhenghan","family":"Zhang","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering Nanjing University  Nanjing 210093 P.R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Luming","family":"Yang","sequence":"additional","affiliation":[{"name":"Research Group ESR Spectroscopy Max Planck Institute for Multidisciplinary Sciences 37077 G\u00f6ttingen Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tianyang","family":"Chen","sequence":"additional","affiliation":[{"name":"Department of Chemical Engineering Stanford University  Stanford CA USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Liu","family":"He","sequence":"additional","affiliation":[{"name":"National Key Laboratory of Advanced Micro and Nano Manufacture Technology Key Laboratory of Polymer Chemistry and Physics of Ministry of Education School of Materials Science and Engineering Peking University  Beijing 100871 P.R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jian","family":"Li","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering Nanjing University  Nanjing 210093 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5072-1952","authenticated-orcid":false,"given":"Maojun","family":"Zheng","sequence":"additional","affiliation":[{"name":"Key Laboratory of Artificial Structure and Quantum Control Ministry of Education School of Physics and Astronomy Shanghai Jiao Tong University  Shanghai 200240 P.R. 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