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Herein, we report a steric\u2010hindrance\u2010driven breaking of interlayer \u03c0\u2013\u03c0 stacking in one\u2010dimensional (1D) COFs built from sterically enforced non\u2010coplanar monomers, thereby rendering the accessibility of aromatic domains and enabling superior adsorption performance, as exemplified by I\n                    <jats:sub>2<\/jats:sub>\n                    uptake. Two COFs, TFPE\u2010MDA, and TFPB\u2010MDA, are assembled via interlayer van der Waals stacking, where the aromatic moieties orient toward the pore channels exposing the backbone \u03c0 electrons; electron population analysis verifies that this packing does not perturb the \u03c0\u2010electron distribution. Iodine\u2010vapor adsorption measurements show high I\n                    <jats:sub>2<\/jats:sub>\n                    uptake capacities of 4.80 and 5.61\u00a0g\u00b7g\n                    <jats:sup>\u22121<\/jats:sup>\n                    for TFPE\u2010MDA and TFPB\u2010MDA, respectively. FTIR, Raman, and XPS characterizations combined with theoretical calculations confirm I\u00b7\u00b7\u00b7\u03c0 interactions between I\n                    <jats:sub>2<\/jats:sub>\n                    and the accessible \u03c0 electrons of aromatic moieties in the COF frameworks. This study provides a novel design strategy for high\u2010performance COF materials by utilizing sterically enforced non\u2010coplanar monomers for breaking the commonly observed interlayer \u03c0\u2013\u03c0 stacking, thus enabling the access and utilization of the intrinsic \u03c0 electrons in COF backbones.\n                  <\/jats:p>","DOI":"10.1002\/anie.3547091","type":"journal-article","created":{"date-parts":[[2026,6,4]],"date-time":"2026-06-04T08:52:12Z","timestamp":1780563132000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Breaking \u03c0\u2013\u03c0 Stacking in One\u2010Dimensional Covalent Organic Frameworks"],"prefix":"10.1002","volume":"65","author":[{"given":"Haoran","family":"Xia","sequence":"first","affiliation":[{"name":"School of Chemistry Southwest Jiaotong University  Chengdu 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Chemistry College of Sciences Northeastern University  Shenyang China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5491-1155","authenticated-orcid":false,"given":"Wei","family":"Zhang","sequence":"additional","affiliation":[{"name":"Department of Chemistry University of Colorado Boulder  Colorado USA"},{"name":"Department of Chemistry Kyung Hee University  Seoul Republic of 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