Abstract. We report in-plume carbon dioxide (CO2) concentrations and isotope ratios during an active eruption of the Tajogaite Volcano. CO2 measurements inform our understanding of volcanic contributions to the global climate carbon cycle, and the role of CO2 in eruptions. Traditional ground-based methods of CO2 collection are difficult and dangerous, as a result only 5 % of volcanoes have been surveyed. We demonstrate that Unpiloted Aerial System (UAS) surveys allow for fast and relatively safe measurements. Using CO2 concentration profiles we estimate total flux to be 1.19 × 106 to 2.80 × 107 t day−1. Isotope ratios indicated a deep magmatic source, consistent with the intensity of the eruption. Our work demonstrates the feasibility of UASs for CO2 surveys during active volcanic eruptions, particularly in calculating plume characteristics.