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Solution\u2010state crystallization\u2010driven self\u2010assembly (CDSA) of CPs into nanowires (NWs) enables solution\u2010processable thin films without post\u2010deposition annealing to enhance crystallinity. In cast films, crystalline NWs provide charge\u2010transport pathways, whereas non\u2010aggregated amorphous chains bridge adjacent NW crystallites, sustain interdomain charge percolation, and accommodate mechanical deformation. Yet this assembly inevitably yields heterogeneous mixtures of crystalline NWs and amorphous chains, which resist single\u2010NW quantification and independent control. In this study, density\u2010driven differential sedimentation fractionates poly(3\u2010hexylthiophene) (P3HT) NWs into a sediment of crystalline NWs and a supernatant of shorter NWs and lower\u2010molecular\u2010weight chains. Cryo\u2010TEM quantitative morphological mapping resolves backbone tilt, width uniformity, and lamellar coherence at the single\u2010NW level, showing that local cofacial \u03c0\u2013\u03c0 packing is preserved in both fractions whereas long\u2010range order along the lamellar stacking direction is concentrated in the sediment. Recombining the fractions at controlled weight ratios tunes the mobility\u2013stretchability trade\u2010off without chemical modification, and the strategy generalizes to coaxial p\u2013n heterojunction hybrid NWs of P3HT\u2010\n                    <jats:italic>b<\/jats:italic>\n                    \u2010poly(2\u2010vinylpyridine)\/CdSe quantum dots formed by CDSA, reframing structural heterogeneity as a programmable design parameter for stretchable electronics.\n                  <\/jats:p>","DOI":"10.1002\/adma.75087","type":"journal-article","created":{"date-parts":[[2026,10,6]],"date-time":"2026-10-06T04:21:57Z","timestamp":1791260517000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Differential Sedimentation and Cryo\u2010TEM Mapping Resolve Structural Heterogeneity in Conjugated Polymer Nanowires for Programmable Stretchable Electronics"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0003-0955-9839","authenticated-orcid":false,"given":"Junyeon","family":"Yoon","sequence":"first","affiliation":[{"name":"Department of Materials Science and Engineering Gwangju Institute of Science and Technology (GIST)  Gwangju Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jun Ho","family":"Hwang","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering Gwangju Institute of Science and Technology (GIST)  Gwangju Republic of Korea"},{"name":"GIST InnoCORE AI\u2010Nano Convergence Institute for Early Detection of Neurodegenerative Diseases Gwangju Institute of Science and Technology (GIST)  Gwangju Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7494-1776","authenticated-orcid":false,"given":"Eunji","family":"Lee","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering Gwangju Institute of Science and Technology (GIST)  Gwangju Republic of Korea"},{"name":"GIST InnoCORE AI\u2010Nano Convergence Institute for Early Detection of Neurodegenerative Diseases Gwangju Institute of Science and Technology (GIST)  Gwangju Republic of Korea"},{"name":"Department of Chemistry Gwangju Institute of Science and Technology (GIST)  Gwangju Republic of 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