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The molecular designs to obtain supramolecular polymers in non\u2010polar and polar solvents are typically orthogonal. Here, we disclose a molecular design in which we combine hydrogen\u2010bonding amide units attached to alkyl chains for compatibility with non\u2010polar solvents and heteroatom in the \u03c0\u2010conjugated core for interaction with polar solvents, leading to supramolecular polymerization of the same monomeric unit in both non\u2010polar and mixture of polar solvents. Redox\u2010active phenazine appended with two amide groups was studied as a model monomeric unit and it undergoes cooperative polymerization via intermolecular hydrogen\u2010bonding resulting in one\u2010dimensional (1D) nanostructures with co\u2010facial type packing in non\u2010polar solvents. Whereas, in a mixture of polar solvents, a\n                    <jats:italic>J<\/jats:italic>\n                    \u2010type packing was observed with tunable morphology from globular to 1D nanostructures based on the polarity of the cosolvent used. Further, solvent isotopic substitution studies suggest that the amphiphilicity of the system can be attributed to the nitrogen\u2010atom in phenazine, which is capable of interacting with polar solvent molecules. Thus, this study opens up azaacenes as a new class of \u03c0\u2010conjugated units for functional supramolecular polymers.\n                  <\/jats:p>","DOI":"10.1002\/anie.202424138","type":"journal-article","created":{"date-parts":[[2025,3,28]],"date-time":"2025-03-28T02:21:50Z","timestamp":1743128510000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":9,"title":["Cooperative Supramolecular Polymerization in Both Polar and Non\u2010Polar Solvents via Heteroatom\u2010Driven Amphiphilicity"],"prefix":"10.1002","volume":"64","author":[{"given":"Sourav","family":"Nandi","sequence":"first","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Bombay  Powai Mumbai 400076 India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Satyabrata","family":"Behera","sequence":"additional","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Bombay  Powai Mumbai 400076 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