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While prior studies emphasize smoother edges as essential for optimal performance, the potential benefits of controlled edge roughness remain largely unexplored. Additionally, most investigations focus on GNR arrays, leaving critical edge\u2010 and width\u2010dependent factors, including fringe fields, bandgap widening, interactions between adsorbing molecules and GNR atoms, density of states (DOS) suppression, and electrostatic screening lengths, and their collective impact on sensitivity, poorly understood. Here, we fabricated field\u2010effect transistors using individual GNRs (widths: 200\u201320\u00a0nm) and characterized their response to molecular adsorption with perfluorooctanoic acid as the model analyte. Narrower ribbons displayed significantly enhanced sensitivity, yielding a coverage\u2010normalized response of 116\u00a0\u00b1\u00a010\u00a0mV per molecule in 20\u00a0nm\u2010wide GNRs (from calibrated ensemble Dirac\u2010point shifts). Experimental and theoretical analyses reveal that this heightened sensitivity arises from stronger fringe fields, width\u2010dependent quantum confinement effects, reduced DOS, and increased edge roughness that facilitates molecular anchoring, enhanced orbital overlap, and improved charge transfer efficiency. Our findings challenge the conventional assumption that smoother edges inherently enhance sensor performance, demonstrating that controlled edge disorder substantially boosts molecular sensitivity in GNR sensors.<\/jats:p>","DOI":"10.1002\/adma.202520102","type":"journal-article","created":{"date-parts":[[2026,1,23]],"date-time":"2026-01-23T08:53:53Z","timestamp":1769158433000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Edge\u2010Driven Fringe\u2010Field Effects, Reduced Screening, and Bandgap Widening in Graphene Nanoribbons Enable Single\u2011Molecule Sensitivity"],"prefix":"10.1002","volume":"38","author":[{"given":"Kavish","family":"Saini","sequence":"first","affiliation":[{"name":"Department of Chemistry and Biochemistry The University of Texas at El Paso  El Paso Texas USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ezra","family":"Bussmann","sequence":"additional","affiliation":[{"name":"Center For Integrated Nanotechnologies Sandia National Laboratories  Albuquerque New Mexico USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Aroop K.","family":"Behera","sequence":"additional","affiliation":[{"name":"Center For Integrated Nanotechnologies Sandia National Laboratories  Albuquerque New Mexico USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Daniel Gomez","family":"Bustos","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Biochemistry The University of Texas at El Paso  El Paso Texas USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Manny de Jesus","family":"Lopez","sequence":"additional","affiliation":[{"name":"Center For Integrated Nanotechnologies Sandia National Laboratories  Albuquerque New Mexico USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Winson C. 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