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The Multiangle Imaging Spectroradiometer (MISR) and the Moderate Resolution Imaging Spectroradiometer (MODIS), launched on 18 December 1999 aboard the Terra spacecraft, are making global observations of top-of-atmosphere (TOA) radiances. Aerosol optical depths and particle properties are independently retrieved from these radiances using methodologies and algorithms that make use of the instruments’ corresponding designs. This paper compares instantaneous optical depths retrieved from simultaneous and collocated radiances measured by the two instruments at locations containing sites within the Aerosol Robotic Network (AERONET). A set of 318 MISR and MODIS images, obtained during the months of March, June, and September 2002 at 62 AERONET sites, were used in this study. The results show that over land, MODIS aerosol optical depths at 470 and 660 nm are larger than those retrieved from MISR by about 35% and 10% on average, respectively, when all land surface types are included in the regression. The differences decrease when coastal and desert areas are excluded. For optical depths retrieved over ocean, MISR is on average about 0.1 and 0.05 higher than MODIS in the 470 and 660 nm bands, respectively. Part of this difference is due to radiometric calibration and is reduced to about 0.01 and 0.03 when recently derived band-to-band adjustments in the MISR radiometry are incorporated. Comparisons with AERONET data show similar patterns.