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Herein, we report a unique example of multistep secondary nucleation\u2010dominated controlled supramolecular polymerization of an amide\u2010functionalized naphthalene monoimide derivative (\n                    <jats:bold>O\u2010NMI\u20101<\/jats:bold>\n                    ) in a methylcyclohexane:decane mixture, undergoing a stepwise transformation from a metastable particle to crystalline nanorods via intermediate nanotapes over 48 h. The resulting hydrogen\u2010bonded nanorods display enhanced emission, a high quantum yield (34%) and strong circularly polarized luminescence (CPL), revealing an unprecedented correlation between their structural evolution and the time\u2010dependent increment in the CPL intensity, reaching an appreciably high luminescence dissymmetry factor (\n                    <jats:italic>g<\/jats:italic>\n                    <jats:sub>lum<\/jats:sub>\n                    ) of \u223c0.088 in the film state. Contrastingly, the seeded polymerization of\n                    <jats:bold>O\u2010NMI\u20101<\/jats:bold>\n                    follows a fragmentation\u2010dominated mechanism, yielding unexpected fragmented nanorods in multi\u2010seeding cycles. Control experiments with a structurally similar analogue (\n                    <jats:bold>O\u2010NMI\u20102<\/jats:bold>\n                    ), lacking a methylene spacer, revealed no CPL, highlighting the spacer's crucial role in controlling the excited\u2010state chiral emission. The contrasting behavior between the two monomers enabled hetero\u2010seeded polymerization of\n                    <jats:bold>O\u2010NMI\u20101<\/jats:bold>\n                    nanorods from\n                    <jats:bold>O\u2010NMI\u20102<\/jats:bold>\n                    fibrillar seeds, producing CPL\u2010active unique heterostructures under kinetic control from two initial CPL\u2010silent components. The present findings unveil the overlooked impact of secondary nucleation in temporal control of supramolecular chirality and CPL\u2010activity in homo\u2010 and heterostructures of supramolecular polymers.\n                  <\/jats:p>","DOI":"10.1002\/smll.202512262","type":"journal-article","created":{"date-parts":[[2026,3,10]],"date-time":"2026-03-10T11:59:21Z","timestamp":1773143961000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Circularly Polarized Luminescence (CPL)\u2010Active Homo\u2010 and Heterostructures by Surface\u2010Catalyzed Secondary Supramolecular Polymerization"],"prefix":"10.1002","volume":"22","author":[{"ORCID":"https:\/\/orcid.org\/0009-0003-9167-056X","authenticated-orcid":false,"given":"Yaiswarya","family":"Das Karmakar","sequence":"first","affiliation":[{"name":"School of Applied and Interdisciplinary Sciences Indian Association for the Cultivation of Science (IACS)  Kolkata West 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