This study compares aerosol optical depths (AOD) products from the Moderate Resolution Imaging Spectroradiometer (MODIS) and the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model and their integrated products with ground measurements across the eastern U.S. from March 1, 2000 to December 31, 2001. The Terra MODIS Level-3 (collection 4) AOD at 0.55 mm has better correlation, but consistently overestimates the values of the Aerosol Robotic Network (AERONET) measurements. GOCART has small biases for a 22-month integration, and slight positive biases appeared for the cold season. These results are also supported by the comparison with the IMPROVE (Interagency Monitoring of Protected Visual Environments) light extinction index. The optimal interpolation improves the daily-scale RMSE from either MODIS or GOCART alone. However, the regional biases in the aerosol products constitute a major constraint to the optimal estimate of AOD.