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To date, however, the development of covalent organic framework (COF)\u2010supported late\u2010transition\u2010metal catalysts has remained unexplored. Herein, we report the facile construction of a heterogeneous Ni@PY\u2010COF catalyst via straightforward coordinated post\u2010synthetic modification of a dipyridyl\u2010functionalized COF. This system delivers highly active (10\n                    <jats:sup>6<\/jats:sup>\n                    \u00a0g mol\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    ) and thermally stable (up to 100\u00b0C) Ni catalytic sites without requiring bulky steric substituents on the ligand. The catalyst produces semicrystalline, predominantly methyl\u2010branched polyethylene featuring high molecular weight (29\u2013297\u00a0kg mol\n                    <jats:sup>\u22121<\/jats:sup>\n                    ), high melting points (121\u00b0C\u2013128\u00b0C), low branching density (\u2264 25\/1000 C), and well\u2010controlled particle morphology. Structural analysis reveals that the confined nanoscale environment of the highly porous COF framework suppresses\n                    <jats:italic>\u03b2<\/jats:italic>\n                    \u2010H elimination, the dominant chain transfer and termination pathway in late\u2010transition\u2010metal\u2010catalyzed olefin polymerization. This work demonstrates the feasibility of integrating late\u2010transition\u2010metal active sites into an atomically precise COF material to enable heterogeneous olefin polymerization rather than oligomerization, thereby establishing a transformative paradigm for advancing high\u2010performance and industrially relevant polyolefin catalysts.\n                  <\/jats:p>","DOI":"10.1002\/anie.4402122","type":"journal-article","created":{"date-parts":[[2026,8,11]],"date-time":"2026-08-11T12:21:10Z","timestamp":1786450870000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Easily Accessible and Highly Active Heterogeneous Nickel Catalyst Supported by Covalent Organic Framework for In Situ Ethylene Polymerization"],"prefix":"10.1002","volume":"65","author":[{"given":"Junhui","family":"Liu","sequence":"first","affiliation":[{"name":"State Key Laboratory of Advanced Fiber Materials College of Materials Science and Engineering Donghua University  Shanghai P. 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