This dataset provides atmospheric concentrations of halocarbons and hydrocarbons measured by the UC-Irvine Whole Air Sampler (WAS) during airborne campaigns conducted by NASA's Atmospheric Tomography (ATom) mission. The analysis of samples from the UCI WAS provides measurements of more than 50 trace gases, including C2-C10 NMHCs, C1-C2 halocarbons, C1-C5 alkyl nitrates, and selected sulfur compounds. Species were identified and measured using an established technique of airborne whole air sampling followed by laboratory analysis using gas chromatography (GC) with flame ionization detection (FID), and mass spectrometric detection (MSD). The ATom mission deployed 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.