Here we discuss the removal of nitrogen dioxide, an important toxic industrial chemical and pollutant, from air using the MOF UiO‐66‐NH2. The amine group is found to substantially aid in the removal, resulting in unprecedented removal capacities upwards of 1.4 g of NO2 /g of MOF. Furthermore, whereas NO2 typically generates substantial quantities of NO on sorbents, the amount generated by UiO‐66‐NH2 is significantly reduced. Of particular significance is the formation of a diazonium ion on the aromatic ring of the MOF, and the potential reduction of NO2 to molecular nitrogen.