This dataset provides information on greenhouse gases and human-produced air pollution, including atmospheric concentrations of carbon dioxide (CO2), methane (CH4), tropospheric ozone (O3), and black carbon (BC) aerosols, collected during airborne campaigns conducted by NASA's Atmospheric Tomography (ATom) mission. This dataset includes merged data from all instruments plus additional data such as numbered profiles and distance flown. Merged data have been created for seven different sampling intervals. In the case of data obtained over longer time intervals (e.g. flask data), the merge files provide (weighted) averages to match the sampling intervals. ATom deploys an extensive gas and aerosol payload on the NASA DC-8 aircraft for a 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. Profiles of the reactive gases will also provide critical information for the validation of satellite data, particularly in remote areas where in situ data is lacking. Complete aircraft flight information including, but not limited to, latitude, longitude, and altitude are also provided. This data release provides results from all instruments on all four ATom flight campaigns.