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Unoccupied aircraft systems (UAS) are developing into fundamental tools for tackling the grand challenges in volcanology; here, we review the systems used and their diverse applications. UAS can typically provide image and topographic data at two orders of magnitude better spatial resolution than space-based remote sensing, and close-range observations at temporal resolutions down to those of video frame rates. Responsive deployments facilitate dense time-series measurements, unique opportunities for geophysical surveys, sample collection from hostile environments such as volcanic plumes and crater lakes, and emergency deployment of ground-based sensors (and robots) into hazardous regions. UAS have already been used to support hazard management and decision-makers during eruptive crises. As technologies advance, increasing system capabilities, autonomy and availability, supported by more diverse and lighter-weight sensors, will offer unparalleled potential for hazard monitoring. UAS will provide opportunities for pivotal advances in our understanding of complex physical and chemical volcanic processes.