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Here, we report a structurally simple series of oligomers with alternating\n                    <jats:italic>ortho<\/jats:italic>\n                    \u2010phenylene and 2,3\u2010pyrazinylene repeat units. Deconvolution of variable\u2010temperature\n                    <jats:sup>1<\/jats:sup>\n                    H NMR spectra, with the help of ab initio chemical shift predictions, shows that the oligomers favor a compact, arene\u2010stacked helix in chloroform but a structurally distinct extended helix in acetone. The longest oligomer investigated, a heptamer, exhibits nearly perfect solvent\u2010switching behavior at low temperature, effectively doubling its length in acetone compared to chloroform. X\u2010ray crystallography confirms that the hybrid backbone is capable of both folding motifs. While arene\u2013arene stacking drives folding in chloroform, nonclassical intramolecular C\u2060\u2500H\u2060\u22ef\u2060N hydrogen bonds appear to be more important in acetone. Both geometries are enthalpically favored in their respective solvents, highlighting how a balance of weak, competing interactions can be harnessed to achieve large\u2010scale geometry changes in synthetic foldamers.\n                  <\/jats:p>","DOI":"10.1002\/chem.71727","type":"journal-article","created":{"date-parts":[[2026,9,25]],"date-time":"2026-09-25T11:56:27Z","timestamp":1790337387000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Foldamers With Two Distinct Helical Motifs Controlled by Solvent"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0007-3393-7675","authenticated-orcid":false,"given":"Yinhui","family":"Liao","sequence":"first","affiliation":[{"name":"Department of Chemistry and Biochemistry Miami University  Oxford Ohio USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9258-1548","authenticated-orcid":false,"given":"Vipul","family":"Batra","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Biochemistry Miami University  Oxford Ohio USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3480-2055","authenticated-orcid":false,"given":"Govinda Prasad","family":"Devkota","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Biochemistry Miami University  Oxford Ohio USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Annabelle","family":"Ryu","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Biochemistry Miami University  Oxford Ohio USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Henry S.","family":"Oliver","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Biochemistry Miami University  Oxford Ohio USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"David L.","family":"Tierney","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Biochemistry Miami University  Oxford Ohio USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5997-6169","authenticated-orcid":false,"given":"C. 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