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Formed under high\u2010temperature conditions (ca. 500\u00b0C\u2013600\u00b0C), these junction\u2010rich architectures are generally resistant to post\u2010synthetic lattice editing or recovery of intact fullerene building blocks. However, we show here that mild transition\u2010metal coordination can unlock these frameworks under mild solution conditions by cleaving covalent intercage C\u2500C bonds. Treating Mg\n                    <jats:sub>4<\/jats:sub>\n                    C\n                    <jats:sub>60<\/jats:sub>\n                    with W(CO)\n                    <jats:sub>4<\/jats:sub>\n                    (Ph\n                    <jats:sub>2<\/jats:sub>\n                    PCH\n                    <jats:sub>2<\/jats:sub>\n                    )\n                    <jats:sub>2<\/jats:sub>\n                    leads to measurable depolymerization and time\u2010dependent formation of molecular C\n                    <jats:sub>60<\/jats:sub>\n                    . NiCl\n                    <jats:sub>2<\/jats:sub>\n                    (PMe\n                    <jats:sub>3<\/jats:sub>\n                    )\n                    <jats:sub>2<\/jats:sub>\n                    promotes substantially more efficient cleavage and enables direct detection of a cleavage intermediate (\n                    <jats:italic>m<\/jats:italic>\n                    \/\n                    <jats:italic>z<\/jats:italic>\n                    \u00a0=\u00a0899), supporting coordination\u2010linked bond\u2010scission pathway. Density functional theory shows that C\n                    <jats:sub>60<\/jats:sub>\n                    \u2013M\u2013C\n                    <jats:sub>60<\/jats:sub>\n                    bridge formation increases the exothermicity for intercage C\u2500C bond scission, and rationalizes the stronger thermodynamic driving force for Ni\u2010catalytic system relative to W\u2010catalytic system. Furthermore, Mg\n                    <jats:sup>2+<\/jats:sup>\n                    removal markedly suppresses depolymerization, indicating that Mg intercalation promotes junction opening through MgCl\n                    <jats:sub>2<\/jats:sub>\n                    formation and charge\u2010state modulation. These results establish coordination\u2010triggered intercage bond cleavage as a strategy for lattice editing and programmable disassembly in carbon\u2010rich 2D frameworks.\n                  <\/jats:p>","DOI":"10.1002\/anie.1816694","type":"journal-article","created":{"date-parts":[[2026,8,26]],"date-time":"2026-08-26T09:41:36Z","timestamp":1787737296000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Coordination\u2010Triggered Disassembly of Robust Two\u2010Dimensional Fullerene Frameworks via Intercage C\u2500C \u03c3\u2010Bond Scission"],"prefix":"10.1002","author":[{"given":"Shuwen","family":"Jia","sequence":"first","affiliation":[{"name":"State Key Laboratory of New Textile Materials and Advanced Processing School of Materials Science and Engineering Huazhong University of Science and Technology  Wuhan 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