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 products have been created for seven different aggregation intervals (1 second, 10 seconds, and 5 instrument-specific 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. 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.