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Herein, a series of symmetric SMAs (\n                    <jats:bold>TC1\u2010F<\/jats:bold>\n                    to\n                    <jats:bold>TC4\u2010F<\/jats:bold>\n                    ) with progressively outward\u2010shifted branching sites and asymmetric\/symmetric counterparts (\n                    <jats:bold>A\u2010TC3\u2010F<\/jats:bold>\n                    and\n                    <jats:bold>TC3\u2010NF<\/jats:bold>\n                    ) incorporating unidirectional\/bidirectional naphthyl\u2010based terminals, are synthesized for efficient binary OSCs. The optimal 3\u02b3\n                    <jats:sup>d<\/jats:sup>\n                    carbon branching site induces a distinct triclinic crystallographic system with closer \u03c0\u2010\u03c0 stacking. Unidirectional naphthyl terminal\u2010based single\u2010crystal creates an unprecedented 2D lamellar network\/3D interpenetrated packing that provides multidimensional charge\u2010transport pathways, which enabled an improved\n                    <jats:italic>L<\/jats:italic>\n                    <jats:sub>D<\/jats:sub>\n                    and electron mobility in\n                    <jats:bold>A\u2010TC3\u2010F<\/jats:bold>\n                    neat film. The\n                    <jats:bold>A\u2010TC3\u2010F<\/jats:bold>\n                    \u2010based blends optimize film formation kinetics and exhibit superior ordered molecular stacking morphology, yielding faster charge transport. Consequently, the optimized\n                    <jats:bold>A\u2010TC3\u2010F<\/jats:bold>\n                    \u2010based binary OSCs achieve a champion PCE of 20.70% and an ultralow \u0394\n                    <jats:italic>E<\/jats:italic>\n                    <jats:sub>3<\/jats:sub>\n                    of 0.191\u00a0eV, setting a new benchmark for binary OSCs with asymmetric terminal\u2010based SMAs. Our systematic work highlights an innovative pathway for precisely tailoring the side\u2010chain branching position and a unidirectional terminal \u03c0\u2010extension strategy to optimize molecular packing, mitigate trade\u2010offs of device parameters, and boost benchmark PCE and minimal \u0394\n                    <jats:italic>E<\/jats:italic>\n                    <jats:sub>3<\/jats:sub>\n                    of binary OSCs with asymmetric terminal\u2010based SMAs.\n                  <\/jats:p>","DOI":"10.1002\/adma.73646","type":"journal-article","created":{"date-parts":[[2026,6,13]],"date-time":"2026-06-13T13:51:36Z","timestamp":1781358696000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":9,"title":["Rational Asymmetric Acceptor Engineering via Unidirectional Terminal \u03c0\u2010Extension and Optimizing Alkyl Branching Sites Affords a Binary Photovoltaic Efficiency\u00a0of 20.7% by Suppressed Nonradiative Energy Loss"],"prefix":"10.1002","volume":"38","author":[{"given":"Heng","family":"Zhang","sequence":"first","affiliation":[{"name":"Key Laboratory of Cluster Science of the Ministry of Education Beijing Key Laboratory of Intelligent Molecular Materials and High\u2010throughput Manufacturing School of Chemistry and Chemical Engineering Beijing Institute of Technology  Beijing P. 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