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Here, we report that surface\u2010emanated micellar brush with a forest\u2010like soft architecture can finely modulate the orientation and microstructure of metal electrodeposition. The poly(\n                    <jats:sc>l<\/jats:sc>\n                    \u2010lactic acid)\u2010b\u2010poly(2\u2010vinylpyridine) micellar brush provides a hierarchically open nanoarray platform for continuous accumulation of metal ions through dynamical coordination with the pyridyl\u2010rich corona and sustained deposition of reduced metal at the inter\u2010micellar voids. Unlike conventional homopolymer coatings that mainly lead to flat deposition of Zn, such micellar\u2010brush layer promotes vertically aligned zinc blades through coupled ion funneling and oriented nanoconfinement. The resulting zinc anode reveals a low nucleation overpotential of \u223c21\u00a0mV, a high Zn\n                    <jats:sup>2+<\/jats:sup>\n                    transference number of 0.79, a rapid rate of \u223c24.2\u00a0\u00b5m h\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 10\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    , and a polarization of only 18\u00a0mV upon reversible plating\/stripping over 3000\u00a0h. The full cells integrated by vertically microstructured Zn anode with V\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>5<\/jats:sub>\n                    cathode retain 89.6% capacity after 1000 cycles at 1 A g\n                    <jats:sup>\u22121<\/jats:sup>\n                    . This work establishes a general route to tailored metal microstructures through softly confined electrodeposition across a spatially directing and chemically associating polymer self\u2010assembly interfaces.\n                  <\/jats:p>","DOI":"10.1002\/anie.5308557","type":"journal-article","created":{"date-parts":[[2026,10,4]],"date-time":"2026-10-04T10:08:46Z","timestamp":1791108526000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Microstructured Metal Electrodeposition at a Micellar Brush\u2010Decorated Interface"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0008-0195-8620","authenticated-orcid":false,"given":"Xiaomin","family":"Cai","sequence":"first","affiliation":[{"name":"School of Chemistry and Chemical Engineering, State Key Laboratory of Synergistic Chem\u2010Bio Synthesis, Frontiers Science Center For Transformative Molecules, State Key Laboratory of Micro\u2010Nano Engineering Science Shanghai Jiao Tong University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhenyan","family":"Ji","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering, State Key Laboratory of Synergistic Chem\u2010Bio Synthesis, Frontiers Science Center For Transformative Molecules, State Key Laboratory of Micro\u2010Nano Engineering Science Shanghai Jiao Tong University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yifan","family":"Zhang","sequence":"additional","affiliation":[{"name":"Shanghai Engineering Research Center of Hierarchical Nanomaterials, Shanghai Key Laboratory of Advanced Polymeric Materials, School of Materials Science and Engineering East China University of Science and Technology  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ming","family":"Sun","sequence":"additional","affiliation":[{"name":"Department of Materials Science Fudan University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiawei","family":"Tao","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering, State Key Laboratory of Synergistic Chem\u2010Bio Synthesis, Frontiers Science Center For Transformative Molecules, State Key Laboratory of Micro\u2010Nano Engineering Science Shanghai Jiao Tong University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4699-6558","authenticated-orcid":false,"given":"Huibin","family":"Qiu","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering, State Key Laboratory of Synergistic Chem\u2010Bio Synthesis, Frontiers Science Center For Transformative Molecules, State Key Laboratory of Micro\u2010Nano Engineering Science Shanghai Jiao Tong University  Shanghai 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