We report the first measurements of volcanic gases with an unmanned aerial vehicle (UAV). The data were collected at La Fossa crater, Vulcano, Italy, during April 2007, with a helicopter UAV of 3 kg payload, carrying an ultraviolet spectrometer for remotely sensing the SO2 flux (8.5 Mg d−1), and an infrared spectrometer, and electrochemical sensor assembly for measuring the plume CO2/SO2 ratio; by multiplying these data we compute a CO2 flux of 170 Mg d−1. Given the deeper exsolution of carbon dioxide from magma, and its lower solubility in hydrothermal systems, relative to SO2, the ability to remotely measure CO2 fluxes is significant, with promise to provide more profound geochemical insights, and earlier eruption forecasts, than possible with SO2 fluxes alone: the most ubiquitous current source of remotely sensed volcanic gas data.