This dataset provides in situ concentrations of nitric oxide (NO), nitrogen dioxide (NO2), total reactive nitrogen oxides (NOy), and ozone (O3) measured by the NOAA Nitrogen Oxides and Ozone (NOyO3) 4-channel chemiluminescence (CL) instrument during airborne campaigns conducted by NASA's Atmospheric Tomography (ATom) mission. NOyO3 provides fast-response, specific, high precision, and calibrated measurements of nitrogen oxides and ozone at a spatial resolution of better than 100 m. ATom deploys an extensive gas and aerosol payload on the NASA DC-8 aircraft for systematic, global-scale sampling of the atmosphere, profiling continuously from 0.2 to 12 km altitude. Flights occurred in each of 4 seasons from 2016 to 2018. Flights originate from the Armstrong Flight Research Center in Palmdale, California, fly north to the western Arctic, south to the South Pacific, east to the Atlantic, north to Greenland, and return to California across central North America. ATom establishes a single, contiguous, global-scale dataset. This comprehensive dataset will be used to improve the representation of chemically reactive gases and short-lived climate forcers in global models of atmospheric chemistry and climate.