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Although the combination of organic and inorganic semiconductors has enabled versatile optoelectronic applications, interlayer coupling in organic\u2013inorganic heterostructures is still limited by inherent material discrepancies such as lattice matching and stacking order. Herein, we demonstrate an interlayer\u2013coupled organic\u2013inorganic heterojunction achieved by interfacial noncovalent F\u00b7\u00b7\u00b7S interactions, which is composed of molecular 5,5''\u2010bis(2\u2010fluorophenyl)\u20102,2':5',2''\u2010terthiophene (oF\u2010PTTTP) and 2D molybdenum disulfide (MoS\n                    <jats:sub>2<\/jats:sub>\n                    ). By leveraging the conformational flexibility afforded by the full C\u2500C single bonds in its backbone, the oF\u2010PTTTP molecules can self\u2010adjust their conformations upon thermal activation. The fluorine atoms on the side chains of oF\u2010PTTTP engage in noncovalent interactions with the sulfur atoms of MoS\n                    <jats:sub>2<\/jats:sub>\n                    at the heterointerface, inducing a pronounced interlayer coupling effect accompanied by lattice strain. This coupling enables near\u2010infrared (NIR) photodetection in a spectral range inaccessible to each individual component, yielding a specific detectivity of 1.8 \u00d7 10\n                    <jats:sup>14<\/jats:sup>\n                    Jones at 808\u00a0nm, which is one of the highest values reported for organic\u2013inorganic heterostructures. Furthermore, the device exhibits gate\u2010tunable positive and negative photoresponses at 808\u00a0nm, allowing real\u2010time motion imaging in the NIR spectrum.\n                  <\/jats:p>","DOI":"10.1002\/adma.202518146","type":"journal-article","created":{"date-parts":[[2026,1,25]],"date-time":"2026-01-25T07:02:47Z","timestamp":1769324567000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Interlayer Coupling in Organic\u2010Inorganic Heterostructures via Interfacial F\u00b7\u00b7\u00b7S Interactions for Near\u2010Infrared Photodetection and Real\u2010Time Motion Recognition"],"prefix":"10.1002","volume":"38","author":[{"given":"Shujing","family":"Guo","sequence":"first","affiliation":[{"name":"State Key Laboratory of Radio Frequency Heterogeneous Integration, and International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education, Institute of Microscale Optoelectronics Shenzhen University Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lei","family":"Zheng","sequence":"additional","affiliation":[{"name":"School of Integrated Circuit Science and Engineering State Key Laboratory of Crystal Materials Tianjin Key Laboratory of Functional Crystal Materials Institute of Functional Crystals Tianjin University of Technology  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yongxu","family":"Hu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Advanced Materials for Intelligent Sensing &amp; Key Laboratory of Organic Integrated Circuit Ministry of Education &amp; Tianjin Key Laboratory of Molecular Optoelectronic Sciences Department of Chemistry, Institute of Molecular Aggregation Science Tianjin University  Tianjin 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Institute of Physics and Chemistry Chinese Academic Society  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ying","family":"Song","sequence":"additional","affiliation":[{"name":"Center for Analysis and Tests Tianjin University  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tao","family":"Xue","sequence":"additional","affiliation":[{"name":"Center for Analysis and Tests Tianjin University  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jinbo","family":"He","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Radio Frequency Heterogeneous Integration, and International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education, Institute of Microscale Optoelectronics Shenzhen University Shenzhen China"},{"name":"State Key Laboratory of Advanced Materials for Intelligent Sensing &amp; Key Laboratory of Organic Integrated Circuit Ministry of Education &amp; Tianjin Key Laboratory of Molecular Optoelectronic Sciences Department of Chemistry, Institute of Molecular Aggregation Science Tianjin University  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yue","family":"Zheng","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Radio Frequency Heterogeneous Integration, and International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education, Institute of Microscale Optoelectronics Shenzhen University Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4841-9287","authenticated-orcid":false,"given":"Cheng","family":"Han","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Radio Frequency Heterogeneous Integration, and International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of 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