This dataset provides atmospheric carbon dioxide (CO2), methane (CH4), carbon monoxide (CO), molecular hydrogen (H2), nitrous oxide (N2O), sulfur hexafluoride (SF6), and other trace gas mole fractions (i.e., concentrations) from airborne campaigns over North America for the NASA Atmospheric Carbon and Transport - America (ACT-America) project. ACT-America's mission spanned five years and included five six-week field campaigns covering all four seasons and three regions of the central and eastern United States. Two instrumented aircraft platforms, the NASA Langley Beechcraft B-200 King Air and the NASA Goddard Space Flight Center's C-130 Hercules, were used to collect high-quality in situ measurements across a variety of continental surfaces and atmospheric conditions. The data were derived from laboratory measurements of whole air samples collected by Programmable Flask Packages (PFP) onboard the two ACT-America aircraft. Approximately 10 - 12 discrete flask samples were captured during each of the 195 flights. This dataset provides results from all five campaigns, including Summer 2016, Winter 2017, Fall 2017, Spring 2018, and Summer 2019.