The ER-2, with the Airborne Visible/Infrared Imaging Spectrometer (AVIRIS) onboard, overflew Rapid City, South Dakota, and the United States Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Site, Oklahoma, on 9 August and 15 August 1993, respectively. High contrast natural and artificial surfaces present in the imagery were used as a basis for retrieving aerosol spectral optical depth (SOD) over these two sites. Coincident measurements of spectral optical depth from a surface-based sunphotometer also were obtained and used as a validation of the AVIRIS derived retrievals. The accuracy of the retrievals is discussed as a function of measurement uncertainty and surface contrast. The results indicate that, given sufficiently small sensor errors and spectrally uniform surfaces with a reflectance difference of at least 0.5, aerosol spectral optical depth over clear continental atmospheres can be retrieved from high spatial resolution space-based imagery to an accuracy of approximately 0.1. Although only two cases are reported here and additional tests are required, these preliminary results suggest that background aerosol spectral optical depth (i.e., τaerosol, <01) cannot be retrieved with adequate accuracy from space; however, the aerosol spectral optical depth of more polluted atmospheres (i.e., τaerosol< 0.2) can be retrieved with adequate accuracy.