We describe the development of Plume Tracker, an interactive toolkit for the analysis of multispectral thermal infrared observations of volcanic plumes and clouds. Plume Tracker is the successor to MAP_SO2, and together these flexible and comprehensive tools have enabled investigators to map sulfur dioxide (SO2) emissions from a number of volcanoes with TIR data from a variety of airborne and satellite instruments. Our objective for the development of Plume Tracker was to improve the computational performance of the retrieval procedures while retaining the accuracy of the retrievals. We have achieved a 300× improvement in the benchmark performance of the retrieval procedures through the introduction of innovative data binning and signal reconstruction strategies, and improved the accuracy of the retrievals with a new method for evaluating the misfit between model and observed radiance spectra. We evaluated the accuracy of Plume Tracker retrievals with case studies based on MODIS and AIRS data acquired over Sarychev Peak Volcano, and ASTER data acquired over Kilauea and Turrialba Volcanoes. In the Sarychev Peak study, the AIRS-based estimate of total SO2 mass was 40% lower than the MODIS-based estimate. This result was consistent with a 45% reduction in the AIRS-based estimate of plume area relative to the corresponding MODIS-based estimate. In addition, we found that our AIRS-based estimate agreed with an independent estimate, based on a competing retrieval technique, within a margin of ±20%. In the Kilauea study, the ASTER-based concentration estimates from 21 May 2012 were within ±50% of concurrent ground-level concentration measurements. In the Turrialba study, the ASTER-based concentration estimates on 21 January 2012 were in exact agreement with SO2 concentrations measured at plume altitude on 1 February 2012.