Abstract Scientific knowledge of transient and difficult-to-access airborne volcanic emissions comes primarily from remote sensing observations, and a few in situ data from sporadic heroic or inadvertent airborne encounters. In the past, patchy knowledge of the composition and behaviour of such plumes from explosive volcanic eruptions, and associated drifting ash and gas clouds, have centrally contributed to unwanted and dangerous aircraft encounters that have put crews at risk and, in some cases, greatly damaged aircraft. Thus, improved knowledge of boundary conditions and plume composition, as inputs to both mass retrieval and predictive models for cloud trajectories , would be of benefit. In this paper, we describe how small robotic unmanned aerial vehicles (sUAVs) can address a variety of measurements that are typically beyond the reach of, and sometimes too dangerous for, manned aircraft. The direct measurements and sampling that can be achieved by sUAVs address serious gaps in knowledge of volcanic processes, and provide important validation data for estimations of volcanogenic ash and gas concentrations gleaned using remote sensing techniques. These data, in turn, constrain key proximal and distal boundary conditions for aerosol and gas transport models on which are based a number of decisions and evaluations by hazard responders and regulatory agencies. We briefly describe a case study from our ongoing field study at Turrialba Volcano in Costa Rica, where we are conducting an international campaign of systematic airborne in situ measurements of volcanogenic SO 2 and other gases, as well as aerosols, with sUAVs and aerostats (e.g. tethered balloons and kites), in conjunction with data acquisitions by the Advanced Spaceborne Thermal Emission and Reflection (ASTER) radiometer onboard the NASA Terra Earth orbital platform. To our knowledge, this is the first such systematic in situ UAV- and aerostat-based observation programme for SO 2 and particulates in a volcanic plume for correlation with orbital data. We preliminarily report good agreement between our UAV/aerostat and ASTER SO 2 retrievals within a 5 km radius of the volcano summit, at altitudes of up to 12 500 ft ( c. 3850 m) above sea level (asl) for concentrations within the range of 5–20 ppmv (ppm by volume). Additional work continues.