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Here, we report a donor\u2010selective templating strategy based on few\u2010layer\u2010like nickel\u2013cobalt layered double hydroxide (NiCo\u2010LDH) nanosheets to regulate polymer donor assembly in OSCs. The hydroxyl\u2010rich NiCo\u2010LDH surface exhibits preferential affinity toward polymer donors and promotes ordered donor\u2010chain organization during film formation, while exerting limited influence on the acceptor component. This templating strategy enhances the molecular ordering of the donor phase and increases the\n                    <jats:italic>L<\/jats:italic>\n                    <jats:sub>D<\/jats:sub>\n                    of D18 from 10.7 to 18.9\u00a0nm, accompanied by the formation of more ordered donor fibrillar structures. The coordinated improvements in donor organization and exciton transport are further associated with enhanced exciton\u2010to\u2010charge conversion, more balanced carrier transport, and suppressed recombination. Consequently, D18:L8\u2010BO\u2010based OSCs achieve a maximum power conversion efficiency (PCE) of 21.36%, independently certified at 21.09%, together with improved stability under continuous illumination. Analogous donor\u2010biased interactions, enhanced exciton diffusion, regulated fibrillar organization, and improved photovoltaic performance are also observed in PM6 and D18\u2010Cl systems. These results highlight the broader applicability of chemically active 2D templating for coordinating polymer donor assembly and exciton transport toward high\u2010performance OSCs.\n                  <\/jats:p>","DOI":"10.1002\/adma.75208","type":"journal-article","created":{"date-parts":[[2026,10,5]],"date-time":"2026-10-05T07:29:56Z","timestamp":1791185396000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Donor\u2010Selective NiCo\u2010LDH Templating Directs Polymer Assembly for Enhanced Exciton Transport in Efficient Organic Solar Cells"],"prefix":"10.1002","author":[{"given":"Yingjie","family":"He","sequence":"first","affiliation":[{"name":"College of Mechanical Engineering &amp; School of Electrical Engineering &amp; School of Nuclear Science and Technology University of South China  Hengyang 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