Conventional SO2 scrubbing agents, namely calcium oxide and zeolites, are often used to remove SO2 using a strong or irreversible adsorption-based process. However, adsorbents capable of sensing and selectively capturing this toxic molecule in a reversible manner, with in-depth understanding of structure-property relationships, have been rarely explored. Here we report the selective removal and sensing of SO2 using recently unveiled fluorinated metal-organic frameworks (MOFs). Mixed gas adsorption experiments were performed at low concentrations ranging from 250 p.p.m. to 7% of SO2. Direct mixed gas column breakthrough and/or column desorption experiments revealed an unprecedented SO2 affinity for KAUST-7 (NbOFFIVE-1-Ni) and KAUST-8 (AlFFIVE-1-Ni) MOFs. Furthermore, MOF-coated quartz crystal microbalance transducers were used to develop sensors with the ability to detect SO2 at low concentrations ranging from 25 to 500 p.p.m.