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However, the development of high\u2010spin\u2010polarization CISS materials still represents a significant challenge. We report the design and preparation of two novel 2D chiral halogen\u2010bonded organic frameworks (XOFs),\n                    <jats:bold>XOF\u2010TPH<\/jats:bold>\n                    and\n                    <jats:bold>XOF\u2010TPO<\/jats:bold>\n                    , constructed from chiral binaphthyl crown ether\u2010based ligands. By modulating the crown ether size, we controlled the molecular flexibility and consequently the crystallinity of the XOFs. The formation of\n                    <jats:bold>XOF\u2010TPH\/TPO<\/jats:bold>\n                    was characterized by\n                    <jats:sup>1<\/jats:sup>\n                    H NMR, XPS, IR, XAFS, PXRD, SAXS, HR\u2010TEM, and SEAD. The frameworks exhibited pronounced Cotton effects and magnetic circular dichroism (CD), confirming their chiral nature.\n                    <jats:bold>XOF\u2010TPH\/TPO<\/jats:bold>\n                    exhibited superior charge\u2010transport capability over the ligands. More importantly, both XOFs demonstrated significantly enhanced CISS effects compared to the monomeric ligands. This enhancement was attributed to the well\u2010ordered framework structures and the heavy\u2010atom effect of iodine, which amplifies spin\u2010orbit coupling. Notably,\n                    <jats:bold>XOF\u2010TPH<\/jats:bold>\n                    , with higher crystallinity, exhibited remarkable CISS performance with a spin polarization up to 94%, implying the crucial role of structural order. This work showed the tremendous potential of chiral XOFs for high spin selectivity and offered valuable insights into the structure\u2013property relationship within CISS, which is crucial for the development of high\u2010performance CISS materials.\n                  <\/jats:p>","DOI":"10.1002\/anie.5989322","type":"journal-article","created":{"date-parts":[[2026,8,20]],"date-time":"2026-08-20T12:25:57Z","timestamp":1787228757000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Supramolecular Chiral Halogen\u2010Bonded Organic Frameworks Enhance Efficient Chirality\u2010Induced Spin Selectivity"],"prefix":"10.1002","volume":"65","author":[{"given":"Congcong","family":"Zhang","sequence":"first","affiliation":[{"name":"The Institute for Advanced Studies Hubei Key Lab On Organic and Polymeric Opto\u2010Electronic Materials Wuhan University  Wuhan Hubei 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Hubei Key Lab On Organic and Polymeric Opto\u2010Electronic Materials Wuhan University  Wuhan Hubei China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Haocheng","family":"Liao","sequence":"additional","affiliation":[{"name":"The Institute for Advanced Studies Hubei Key Lab On Organic and Polymeric Opto\u2010Electronic Materials Wuhan University  Wuhan Hubei China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Pengju","family":"Tian","sequence":"additional","affiliation":[{"name":"Key Lab of Functional Polymers For Sustainability of Jiangsu School of Energy and Environment Southeast University  Nanjing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Junyu","family":"Zhang","sequence":"additional","affiliation":[{"name":"The Institute for Advanced Studies Hubei Key Lab On Organic and Polymeric Opto\u2010Electronic Materials Wuhan University  Wuhan Hubei 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