A metal-organic framework (MOF) material was developed that exhibits a selective, fully reversible, and repeatable capability to remove nitrogen dioxide gas from the atmosphere in ambient conditions. The material denoted as MFM-300 (Al) exhibited the first reversible, selective capture of nitrogen dioxide at ambient pressures and temperatures — at low concentrations — in the presence of moisture, sulfur dioxide, and carbon dioxide. Despite the highly reactive nature of nitrogen dioxide, the MFM-300(Al) material proved extremely robust, demonstrating the capability to be fully regenerated, or degassed, multiple times without loss of crystallinity or porosity. Other different porous materials often showed degraded performance in subsequent cycles by the nitrogen dioxide, or that the regeneration process was too difficult and costly.