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Conventional approaches employ either bottom\u2010up chiral small molecule self\u2010assembly or top\u2010down co\u2010assembly of achiral luminophores with supramolecular chiral templates (e.g., cellulose nanocrystals (CNCs), liquid crystals). These templates act as pre\u2010engineered \u201cmolds\u201d to align achiral emitters within chiral matrices. However, co\u2010assembling chiral small molecules with such templates remains underexplored, challenged by complex protocols and limited assembly control, raising fundamental questions about supramolecular chiral interplay. Herein, we elucidate the co\u2010assembly and interplay between chiral aggregation\u2010induced emission (AIE) molecules (PN\u2010Phe halides) and CNCs. Halide ions (F\n                    <jats:sup>\u2013<\/jats:sup>\n                    , Cl\n                    <jats:sup>\u2013<\/jats:sup>\n                    , Br\n                    <jats:sup>\u2013<\/jats:sup>\n                    , and PF\n                    <jats:sub>6<\/jats:sub>\n                    <jats:sup>\u2013<\/jats:sup>\n                    ) profoundly modulate PN\u2010Phe self\u2010assembly, dictating distinct morphologies, packing, chiroptical signals, fluorescent quantum yields (QY), and lifetimes. PN\u2010Phe\u2010Cl\n                    <jats:sup>\u2013<\/jats:sup>\n                    exhibits the highest\n                    <jats:italic>g<\/jats:italic>\n                    <jats:sub>lum<\/jats:sub>\n                    (\u22124.1 \u00d7 10\n                    <jats:sup>\u22123<\/jats:sup>\n                    ), versus PN\u2010Phe\u2010Br\n                    <jats:sup>\u2013<\/jats:sup>\n                    (\u22122.8 \u00d7 10\n                    <jats:sup>\u22123<\/jats:sup>\n                    ). Strikingly, co\u2010assembly into CNC\u2010PVA\u2010PN\u2010Phe\u2010X\u2010 (CPP\u2010X\u2010) composite films reverse this trend: CPP\u2010Cl\n                    <jats:sup>\u2013<\/jats:sup>\n                    achieves an exceptional\n                    <jats:italic>g<\/jats:italic>\n                    <jats:sub>lum<\/jats:sub>\n                    of \u22120.43, contrasting sharply with CPP\u2010Cl\n                    <jats:sup>\u2013<\/jats:sup>\n                    (\u22123.1 \u00d7 10\n                    <jats:sup>\u22122<\/jats:sup>\n                    ). The multiple color variations and potential application in anti\u2010counterfeiting demonstrate the advantages of this co\u2010assembly strategy. This work highlights the significant role of assembly patterns in constructing advanced CPL materials, revealing that halide ions could serve as effective modulators for CPL.\n                  <\/jats:p>","DOI":"10.1002\/smll.202502383","type":"journal-article","created":{"date-parts":[[2025,6,17]],"date-time":"2025-06-17T08:25:31Z","timestamp":1750148731000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":7,"title":["Halide Ion\u2010Modulated Chiral Synergy in Co\u2010Assembled AIEgen\u2010CNC Composites for Circularly Polarized Luminescence"],"prefix":"10.1002","volume":"21","author":[{"given":"Juan","family":"Shao","sequence":"first","affiliation":[{"name":"Research Center for Analytical Sciences Department of Chemistry College of Sciences Northeastern University  Shenyang 110819 P. R. 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