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However, in two\u2010dimensional (2D) material\u2010based sensors, unintended adsorption, particularly of water molecules, often disrupts these interactions, degrading selectivity and long\u2010term stability. Here, we exploit molecular confinement within van der Waals (vdW) gaps of MoS\n                    <jats:sub>2<\/jats:sub>\n                    to engineer sensor\u2013analyte interactions. Ethanol (EtOH) confinement induces electron doping and hydrophobicity, whereas water confinement produces negligible doping and hydrophilicity. This combined modulation suppresses H\n                    <jats:sub>2<\/jats:sub>\n                    O adsorption while promoting selective NO\n                    <jats:sub>2<\/jats:sub>\n                    adsorption, enabling the EtOH\u2010confined sensor to detect NO\n                    <jats:sub>2<\/jats:sub>\n                    from 200 ppb to 5\u00a0ppm, with a maximum response of 48% at 60% relative humidity and a detection limit of 36 ppb. Under highly humid conditions, it exhibits a sevenfold higher NO\n                    <jats:sub>2<\/jats:sub>\n                    response and retains 95% of its initial response after 5 weeks, compared with 44% for H\n                    <jats:sub>2<\/jats:sub>\n                    O\u2010confined films. First\u2010principles calculations reveal that molecular confinement regulates sulfur\u2010vacancy (V\n                    <jats:sub>s<\/jats:sub>\n                    ) configurations: EtOH favors isolated and lined V\n                    <jats:sub>s<\/jats:sub>\n                    , which promote NO\n                    <jats:sub>2<\/jats:sub>\n                    adsorption while suppressing H\n                    <jats:sub>2<\/jats:sub>\n                    O binding, whereas H\n                    <jats:sub>2<\/jats:sub>\n                    O stabilizes clustered V\n                    <jats:sub>s<\/jats:sub>\n                    , which increase H\n                    <jats:sub>2<\/jats:sub>\n                    O affinity. This vdW\u2010gap confinement provides a design strategy to tune surface chemistry, electronic structure, and defect configurations for selective, humidity\u2010tolerant, and reliable 2D chemical sensors.\n                  <\/jats:p>","DOI":"10.1002\/advs.78072","type":"journal-article","created":{"date-parts":[[2026,10,9]],"date-time":"2026-10-09T03:15:03Z","timestamp":1791515703000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Van der Waals Gap\u2010Confined Molecular Engineering of MoS\n                    <sub>2<\/sub>\n                    for Selectivity\u2010Enhanced and Humidity\u2010Tolerant Gas Sensing"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-0253-006X","authenticated-orcid":false,"given":"Jae Hyung","family":"Shim","sequence":"first","affiliation":[{"name":"Department of Electrical and Computer Engineering Seoul National University  Seoul Republic of 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Seoul National University  Seoul Republic of Korea"},{"name":"Inter\u2010University Semiconductor Research Center (ISRC) Seoul National University  Seoul Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jin Seok","family":"Kim","sequence":"additional","affiliation":[{"name":"Department of Electrical and Computer Engineering Seoul National University  Seoul Republic of Korea"},{"name":"Inter\u2010University Semiconductor Research Center (ISRC) Seoul National University  Seoul Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5517-2630","authenticated-orcid":false,"given":"Jung\u2010Won","family":"An","sequence":"additional","affiliation":[{"name":"Electronic and Hybrid Materials Research Center Korea Institute of Science and Technology (KIST)  Seoul Republic of Korea"},{"name":"Department of Materials Science and Engineering Seoul National University  Seoul Republic of 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