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In this work, a ligand extension strategy combined with a controlled etching process is employed in designing and synthesizing zirconium\u2010based MOFs (Zr\u2010MOFs). These structural optimizations increase active sites exposure and improve accessibility to \u03c0\u2010conjugated transport channels. The obtained tetraphenylethylene\u2010based Zr\u2010MOFs exhibit excellent iodine adsorption capacity and strong confinement of polyiodides, enabling their use as cathode hosts in aqueous zinc\u2010iodine batteries. The \u03c0\u2010conjugated tetraphenylethylene ligand further increases the capacitance of batteries by promoting rapid electron dispersion and charge storage within the extended conjugated frameworks. In situ Raman spectroscopy and theoretical analyses reveal that the combination of physical confinement and chemical absorbance effects effectively stabilizes iodine species and governs the charge\u2010discharge mechanism. As a result, the M4\/I\n                    <jats:sub>2<\/jats:sub>\n                    cathode exhibits excellent cycling stability, high multiplicity capacity, and reversible iodine redox kinetics. This research provides a generalizable strategy for constructing MOFs with controlled morphology and structure, offering new insights for the design of future high\u2010performance aqueous battery systems.\n                  <\/jats:p>","DOI":"10.1002\/adma.72860","type":"journal-article","created":{"date-parts":[[2026,3,21]],"date-time":"2026-03-21T10:46:29Z","timestamp":1774089989000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":21,"title":["Tetraphenylethylene\u2010Functionalized Zirconium Metal\u2010Organic Frameworks Enabling Polyiodide Confinement for High\u2010Performance Zinc\u2010Iodine Batteries"],"prefix":"10.1002","volume":"38","author":[{"given":"Chenhui","family":"Yin","sequence":"first","affiliation":[{"name":"School of Chemistry and Materials Yangzhou University  Yangzhou Jiangsu P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaotian","family":"Guo","sequence":"additional","affiliation":[{"name":"School of Chemistry and Materials Yangzhou University  Yangzhou Jiangsu P. R. China"},{"name":"School of Green and Low\u2010Carbon Engineering Yancheng Teachers University  Yancheng P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinyu","family":"Qin","sequence":"additional","affiliation":[{"name":"School of Chemistry and Materials Yangzhou University  Yangzhou Jiangsu P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jia","family":"Shi","sequence":"additional","affiliation":[{"name":"School of Chemistry and Materials Yangzhou University  Yangzhou Jiangsu P. R. China"},{"name":"School of Chemistry and Chemical Engineering Chongqing University of Science and Technology  Chongqing P. R. 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University of Saskatchewan  Saskatoon Canada"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bin","family":"He","sequence":"additional","affiliation":[{"name":"Zhejiang Key Laboratory For Industrial Solid Waste Thermal Hydrolysis Technology and Intelligent Equipment Huzhou Key Laboratory of Environmental Functional Materials and Pollution Control Department of Materials Engineering Huzhou University  Huzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0000-3016-6915","authenticated-orcid":false,"given":"Huijie","family":"Zhou","sequence":"additional","affiliation":[{"name":"School of Chemistry and Materials Yangzhou University  Yangzhou Jiangsu P. R. China"},{"name":"Institute of Technology for Carbon Neutralization Yangzhou University  Yangzhou Jiangsu P. R. 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