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Here, we construct a single\u2010stranded DNA (ssDNA)\u2010directed nanodevice that achieves 94.3% quenching efficiency by harnessing asymmetric \u03c0\u2013\u03c0 interactions to split exciton energy levels. DNA spatial confinement orchestrates hydrophobic, covalent, and \u03c0\u2013\u03c0 interactions, enabling precise component arrangement. This nanodevice comprises a light\u2010harvesting engine, a vibrational metal nanocluster actuator and a programmable ssDNA. Asymmetric \u03c0\u2013\u03c0 interactions between fluorophore and metal nanocluster in DNA spatial confinements split fluorophore energy levels, directing exciton flux. Complementary DNA strands modulate engine\u2010actuator coupling, enabling enthalpy\u2010driven switching between radiative and non\u2010radiative pathways. By tuning DNA length and nanocluster ligands, we achieve continuous control over energy transfer efficiency. This programmable platform, manipulating non\u2010radiative decay via \u03c0\u2013\u03c0 interactions, establishes vibrational control as a general paradigm for nanoscale energy transduction.<\/jats:p>","DOI":"10.1002\/anie.202525693","type":"journal-article","created":{"date-parts":[[2026,2,4]],"date-time":"2026-02-04T04:46:44Z","timestamp":1770180404000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Harnessing Exciton Flux With a Single\u2010Stranded DNA\u2010Programmed Nanodevice"],"prefix":"10.1002","volume":"65","author":[{"given":"Mulin","family":"Duan","sequence":"first","affiliation":[{"name":"State Key Laboratory of Synergistic Chem\u2010Bio Synthesis School of Chemistry and Chemical Engineering New Cornerstone Science Laboratory Frontiers Science Center for Transformative Molecules and National Center for Translational Medicine Shanghai Jiao Tong University  Shanghai 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