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Here, we show that this preference can be overcome through hydrogen\u2010bond\u2010induced switching of the interaction hierarchy governing supramolecular assembly. In croconaine\u2010based dipolar D\u2013A chromophores, the introduction of directional amide\u2010mediated hydrogen bonding establishes a thermodynamically favored homo\u2010association that overrides dipolar complementarity, thereby switching the preferred packing mode from hetero\u2010 to homo\u2010organization. This interaction hierarchy switching drives cooperative homochiral assembly and enables amplified NIR chiroptical responses. Integration of these assemblies into heterojunction devices translates the supramolecular structural reorganization into helicity\u2010dependent electrical outputs, affording efficient NIR circularly polarized photodetection. These results identify interaction hierarchy inversion as an effective strategy for controlling association modes and chiroptical functions in dipolar chromophores.<\/jats:p>","DOI":"10.1002\/anie.1147827","type":"journal-article","created":{"date-parts":[[2026,7,25]],"date-time":"2026-07-25T04:09:53Z","timestamp":1784952593000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Hydrogen\u2010Bond\u2010Induced Switching of Interaction Hierarchy in Dipolar D\u2013A Chromophores for NIR Circularly Polarized Photodetection"],"prefix":"10.1002","volume":"65","author":[{"given":"Laiwei","family":"Gao","sequence":"first","affiliation":[{"name":"State Key Laboratory of Precision and Intelligent Chemistry Department of Polymer Science and Engineering University of Science and Technology of China  Hefei Anhui P. R. 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