This data set provides atmospheric carbon dioxide (CO2), methane (CH4), carbon monoxide (CO), ozone (O3), and water vapor (H2O) concentrations from airborne campaigns over the Alaskan and Canadian arctic for the Carbon in Arctic Reservoirs Vulnerability Experiment (CARVE). These data are merged and gap-filled outputs from two different cavity ring-down spectrometers (CRDS; Picarro Inc.) flown aboard the CARVE aircraft and are presented at 5-second intervals throughout each flight. Aircraft latitude, longitude, and altitude are also provided. 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 content. 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.