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We report that metal-organic frameworks (MOFs) with ligand spin immobilization demonstrate superior chemispintronic sensitivity and selectivity toward nitric oxide. Tetrathiafulvalene radical cations (TTF\u00b7\n            <jats:sup>+<\/jats:sup>\n            ) within the MOF lattice considerably enhance the nitric oxide recognition via spin exchange interactions, leading to a five\u2013order of magnitude reduction in the limit of detection (LOD), as compared to volatile organic compounds (VOCs) via carrier-doping mechanism. Record-low LOD of 0.12\u00a0parts per billion was achieved in M-TTF-spin (M\u00a0=\u00a0cobalt, zinc, and cadmium) MOFs, which also demonstrates exceptional selectivity over typical nitrogen oxides (NO\n            <jats:italic>\n              <jats:sub>x<\/jats:sub>\n            <\/jats:italic>\n            ) and VOCs. This work opens up a distinct sensing platform for radical-like analytes through strategic design of spin-immobilized molecular functional motifs toward the spintronic device configurations.\n          <\/jats:p>","DOI":"10.1126\/sciadv.adq3554","type":"journal-article","created":{"date-parts":[[2025,4,2]],"date-time":"2025-04-02T20:33:04Z","timestamp":1743625984000},"update-policy":"https:\/\/doi.org\/10.34133\/aaas_crossmark","source":"Crossref","is-referenced-by-count":12,"title":["Ligand spin immobilization in metal-organic frameworks enables high-performance chemispintronic detection of radical gas molecules"],"prefix":"10.1126","volume":"11","author":[{"ORCID":"https:\/\/orcid.org\/0009-0002-1564-0046","authenticated-orcid":true,"given":"Cheng","family":"Liu","sequence":"first","affiliation":[{"name":"Key Laboratory of Mesoscopic Chemistry, State Key Laboratory of Coordination Chemistry, State Key Laboratory of Analytical Chemistry for Life Sciences, School of Chemistry and 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