An extensive set of airborne and satellite observations of volcanic ash from the Eyjafjallajökull Icelandic eruption are analyzed for a case study on 17 May 2010. Data collected from particle scattering probes and backscatter lidar on the Facility for Airborne Atmospheric Measurements (FAAM) BAe 146 aircraft allow estimates of ash concentration to be derived. Using radiative transfer simulations we show that airborne and satellite infrared radiances can be accurately modeled based on the in situ measured size distribution and a mineral dust refractive index. Furthermore, airborne irradiance measurements in the 0.3–1.7 μm range are well modeled with these properties. Retrievals of ash mass column loading using Infrared Atmospheric Sounding Interferometer (IASI) observations are shown to be in accord with lidar-derived mass estimates, giving for the first time an independent verification of a hyperspectral ash variational retrieval method. The agreement of the observed and modeled solar and terrestrial irradiances suggests a reasonable degree of radiative closure implying that the physical and optical properties of volcanic ash can be relatively well constrained using data from state-of-the-science airborne platforms such as the FAAM BAe 146 aircraft. Comparisons with IASI measurements during recent Grímsvötn and Puyehue volcanic eruptions demonstrate the importance of accurately specifying the refractive index when modeling the observed spectra.