We introduce and evaluate an approach for the simultaneous retrieval of aerosol and surface properties from Airborne Visible/Infrared Imaging Spectrometer Classic (AVIRIS-C) data collected during wildfires. The joint National Aeronautics and Space Administration/National Oceanic and Atmospheric Administration (NASA/NOAA) Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) field campaign took place in August 2019, and involved two aircraft and coordinated ground-based observations. The AVIRIS-C instrument acquired data from onboard NASA’s high altitude ER-2 research aircraft, coincident in space and time with aerosol observations obtained from the Aerosol Robotic Network (AERONET) DRAGON mobile platform in the smoke plume downwind of the Williams Flats Fire in northern Washington in August, 2019. Observations in this smoke plume were used to assess the capacity of optimal-estimation based retrievals to simultaneously estimate aerosol optical depth (AOD) and surface reflectance from Visible Shortwave Infrared (VSWIR) imaging spectroscopy. Radiative transfer modeling of the sensitivities in spectral information collected over smoke reveal the potential capacity of high spectral resolution retrievals to distinguish between sulfate and smoke aerosol models, as well as sensitivity to the aerosol size distribution. Comparison with ground-based AERONET observations demonstrates that AVIRIS-C retrievals of AOD compare favorably with direct sun AOD measurements. Our analyses suggest that spectral information collected from the full VSWIR spectral interval, not just the shortest wavelengths, enables accurate retrievals. We use this approach to continuously map both aerosols and surface reflectance at high spatial resolution across heterogeneous terrain, even under relatively high AOD conditions associated with wildfire smoke.