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Here, a strategy is provided to tailor the polymer aggregation and their responsiveness to solution\u2010shearing forces by tuning intermolecular interactions, aiming for efficient charge transport. Using a typical n\u2010type conjugated polymer as the model system, we systematically modulate the balance between backbone\u2013solvent and side chain\u2013solvent interactions to design distinct aggregate structures. In the backbone\u2010selective solvent of 1\u2010chloronaphthalene, enhanced backbone solvation at elevated temperatures leads to loosely packed, rod\u2010like aggregates that align efficiently under directional shear, yielding highly ordered films with electron mobilities up to 4.74\u00a0cm\n                    <jats:sup>2<\/jats:sup>\n                    V\n                    <jats:sup>\u22121<\/jats:sup>\n                    s\n                    <jats:sup>\u22121<\/jats:sup>\n                    . In contrast, in the side\u2010chain\u2010selective solvent of trimethylbenzene, polymer chains form disordered network\u2010like aggregates that resist alignment and produce less ordered films with mobilities of 2.20 cm\n                    <jats:sup>2<\/jats:sup>\n                    V\n                    <jats:sup>\u22121<\/jats:sup>\n                    s\n                    <jats:sup>\u22121<\/jats:sup>\n                    . Additionally, similar enhancements in charge\u2010transport mobility are also observed with two other representative polymers using the same strategy. This work establishes the critical role of intermolecular interaction\u2010driven aggregate design in dictating shearing\u2010induced structural evolution, offering a robust framework for the fabrication of high\u2010mobility conjugated polymer films.\n                  <\/jats:p>","DOI":"10.1002\/adma.202521831","type":"journal-article","created":{"date-parts":[[2026,2,21]],"date-time":"2026-02-21T12:54:38Z","timestamp":1771678478000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Tuning Solution\u2010State Aggregation for Shearing\u2010Induced Alignment and High Mobility Transport in Conjugated Polymers"],"prefix":"10.1002","volume":"38","author":[{"given":"Yu\u2010Chun","family":"Xu","sequence":"first","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences (BNLMS) Key Laboratory of Polymer Chemistry and Physics of Ministry of Education Center for Soft Matter Science and Engineering College of Chemistry and Molecular Engineering Peking University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yang\u2010Yang","family":"Zhou","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences (BNLMS) Key Laboratory of Polymer Chemistry and Physics of Ministry of Education Center for Soft Matter Science and Engineering College of Chemistry and Molecular Engineering Peking University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Li","family":"Ding","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences (BNLMS) Key Laboratory of Polymer Chemistry and Physics of Ministry of Education Center for Soft Matter Science and Engineering College of Chemistry and Molecular Engineering Peking University  Beijing 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