This data set provides atmospheric carbon dioxide (CO2), methane (CH4), and carbon monoxide (CO) concentrations from airborne campaigns over the Alaskan and Canadian arctic for the Carbon in Arctic Reservoirs Vulnerability Experiment (CARVE). The data were collected in situ using a four-species cavity ring-down spectrometer system (CRDS; Picarro Inc.) provided by Harvard University and are presented at 5-second intervals throughout each flight. The Harvard CRDS instrument only collected data in 2012-2014; no Harvard data are available for year 2015. Aircraft latitude, longitude, and altitude are also provided. 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 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.