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Herein, we report the characterization at various scales of the assembly properties of a\n                    <jats:italic>C<\/jats:italic>\n                    <jats:sub>2<\/jats:sub>\n                    \u2010symmetric benzene\u20101,3,5\u2010tricarboxamide monomer with two (1\n                    <jats:italic>S<\/jats:italic>\n                    )\u2010methylheptyl moieties and one diphenylphosphino group as lateral chains. Our investigation reveals a highly cooperative structural transition between two SP states, which can exquisitely be tuned by solvents of similar polarities, leading to variation of the transition temperature (T*) over a range of 85\u00a0K. The structural transition was detected in 4 pure solvents and 13 toluene\/cosolvent mixtures; a fair relationship is determined between T* and the solvent molar volume. The transition is only weakly favored by enthalpy (by ca. 2\u00a0kJ.mol\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 286\u00a0K). However, minimization of the entropic cost leads to a notable increase in the T*. This allows a fine tuning of the thermothickening and catalytic properties of the resulting SPs auguring that solvation, and notably solvation entropy, may constitute an important lever for steering SPs structure and properties.\n                  <\/jats:p>","DOI":"10.1002\/anie.202521365","type":"journal-article","created":{"date-parts":[[2025,11,21]],"date-time":"2025-11-21T06:52:41Z","timestamp":1763707961000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":5,"title":["Solvation Entropy as a Lever for Steering the Macroscopic Properties of a Functional Supramolecular Helical Polymer"],"prefix":"10.1002","volume":"65","author":[{"given":"Huanjun","family":"Kong","sequence":"first","affiliation":[{"name":"Sorbonne Universit\u00e9 CNRS Institut Parisien de Chimie Mol\u00e9culaire  4 Place Jussieu Paris 75005 France"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Mayte 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