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In this study, we have developed an effective strategy for programming the pathways of \u03c0\u2010conjugated supramolecular polymers, by incorporating both electron\u2010rich methoxy\u2010 or methanthiol\u2010benzene as donor unit and electron\u2010poor cyano\u2010vinylenes as acceptor units on the monomeric structure. It leads to the formation of parallel\u2010stacked supramolecular polymers as the metastable species through homomeric donor\/acceptor packing, which convert to slip\u2010stacked supramolecular polymers as the thermodynamically stable species facilitated by heteromeric donor\u2010acceptor packing. By further investigating the external seed\u2010induced kinetic\u2010to\u2010thermodynamic transformation behaviors, our findings suggest that the donor\u2010acceptor functionality on the seed structure is crucial for accelerating pathway conversion. This is achieved by eliminating the initial lag phase in the supramolecular polymerization process. Overall, this study provides valuable insights into designing molecular structures that control aggregation pathways of \u03c0\u2010conjugated nanostructures.<\/jats:p>","DOI":"10.1002\/anie.202305827","type":"journal-article","created":{"date-parts":[[2023,7,11]],"date-time":"2023-07-11T06:39:47Z","timestamp":1689057587000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":58,"title":["Pathway Control of \u03c0\u2010Conjugated Supramolecular Polymers by Incorporating Donor\u2010Acceptor Functionality"],"prefix":"10.1002","volume":"62","author":[{"given":"Fan","family":"Wang","sequence":"first","affiliation":[{"name":"Key Laboratory of Precision and Intelligent Chemistry Department of Polymer Science and Engineering University of Science and Technology of China  Hefei Anhui 230026 P. R. 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