This data set 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 the Alaskan and Canadian Arctic for the Carbon in Arctic Reservoirs Vulnerability Experiment (CARVE). The CARVE flight campaigns took place from 2012 to 2015 between the months of March and November to enable investigation of both seasonal and inter-annual variability in atmospheric gas abundances. The data were derived from laboratory measurements of whole air samples collected by a Programmable Flask Package (PFP) onboard the CARVE aircraft. Air samples were collected at strategic intervals to coincide with the overflight of a ground site of interest, or when interesting geophysical conditions were encountered. While most of these samples were collected near the surface in the planetary boundary layer (PBL), on almost every flight samples were also collected in the free troposphere. A minimum of 12 flask samples were collected per flight. Whole air samples collected in the PFPs were analyzed on automated systems at the NOAA Earth System Research Laboratory (ESRL) Global Monitoring Division in Boulder, CO, which also analyzes samples from the NOAA/ESRL Global Greenhouse Gas Reference Network. The measurements included in this data set are crucial for understanding changes in Arctic carbon cycling and the potential threats posed by thawing of Arctic permafrost.