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Here, we report the first single\u2010crystal structures of two imidazole\u2010based dimeric NFAs, revealing well\u2010defined intramolecular \u03c0\u2013\u03c0 stacking and compact molecular packing in the monomolecular state. These structural features lead to shorter \u03c0\u2013\u03c0 stacking distances and enhanced electronic coupling compared to their monomeric counterpart, resulting in improved charge carrier mobility and photoresponse. By varying the length of the alkyl linker, we tailor the optoelectronic properties and suppress the dark current in organic photodetectors (OPDs), enhancing both external quantum efficiency and specific detectivity. Devices based on the C8\u2010linked dimer (H2\u2010C8) achieve a peak detectivity (\n                    <jats:italic>D<\/jats:italic>\n                    <jats:sub>sh<\/jats:sub>\n                    <jats:sup>*<\/jats:sup>\n                    ) of 2.1\u00a0\u00d7\u00a010\n                    <jats:sup>14<\/jats:sup>\n                    Jones at 880\u00a0nm, and maintain values above 3.3\u00a0\u00d7\u00a010\n                    <jats:sup>13<\/jats:sup>\n                    Jones across 340\u2013960\u00a0nm with an ultra\u2010fast photoresponse time of 1.94 (\n                    <jats:italic>t<\/jats:italic>\n                    <jats:sub>rise<\/jats:sub>\n                    ) and 2.11 (\n                    <jats:italic>t<\/jats:italic>\n                    <jats:sub>fall<\/jats:sub>\n                    ) \u00b5s. These figures of merit place H2\u2010C8 among the best\u2010performing self\u2010powered near\u2010infrared OPDs, with performance on par with commercial silicon photodiodes. Our findings provide direct structural insights into dimeric NFAs and establish a new design pathway for high\u2010performance organic optoelectronic materials.\n                  <\/jats:p>","DOI":"10.1002\/anie.202519630","type":"journal-article","created":{"date-parts":[[2025,10,29]],"date-time":"2025-10-29T14:17:05Z","timestamp":1761747425000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Decoding Molecular Conformations of Dimeric Non\u2010Fullerene Acceptors for High\u2010Sensitivity Near\u2010Infrared Organic Photodetectors"],"prefix":"10.1002","volume":"64","author":[{"given":"Hanjian","family":"Lai","sequence":"first","affiliation":[{"name":"Shenzhen Grubbs Institute and Department of Chemistry Southern University of Science and Technology  1088 Xueyuan Blvd., Nanshan District Shenzhen Guangdong 518055 P. R. China"},{"name":"School of Electrical Engineering University of South China  Hengyang 421001 P. 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