Abstract The Chesapeake Lighthouse Aircraft Measurements for Satellites (CLAMS) experiment took place from 10 July to 2 August 2001 in a combined ocean–land region that included the Chesapeake Lighthouse [Clouds and the Earth’s Radiant Energy System (CERES) Ocean Validation Experiment (COVE)] and the Wallops Flight Facility (WFF), both along coastal Virginia. This experiment was designed mainly for validating instruments and algorithms aboard the Terra satellite platform, including the Moderate Resolution Imaging Spectroradiometer (MODIS). Over the ocean, MODIS retrieved aerosol optical depths (AODs) at seven wavelengths and an estimate of the aerosol size distribution. Over the land, MODIS retrieved AOD at three wavelengths plus qualitative estimates of the aerosol size. Temporally coincident measurements of aerosol properties were made with a variety of sun photometers from ground sites and airborne sites just above the surface. The set of sun photometers provided unprecedented spectral coverage from visible (VIS) to the solar near-infrared (NIR) and infrared (IR) wavelengths. In this study, AOD and aerosol size retrieved from MODIS is compared with similar measurements from the sun photometers. Over the nearby ocean, the MODIS AOD in the VIS and NIR correlated well with sun-photometer measurements, nearly fitting a one-to-one line on a scatterplot. As one moves from ocean to land, there is a pronounced discontinuity of the MODIS AOD, where MODIS compares poorly to the sun-photometer measurements. Especially in the blue wavelength, MODIS AOD is too high in clean aerosol conditions and too low under larger aerosol loadings. Using the Second Simulation of the Satellite Signal in the Solar Spectrum (6S) radiative code to perform atmospheric correction, the authors find inconsistency in the surface albedo assumptions used by the MODIS lookup tables. It is demonstrated how the high bias at low aerosol loadings can be corrected. By using updated urban/industrial aerosol climatology for the MODIS lookup table over land, it is shown that the low bias for larger aerosol loadings can also be corrected. Understanding and improving MODIS retrievals over the East Coast may point to strategies for correction in other locations, thus improving the global quality of MODIS. Improvements in regional aerosol detection could also lead to the use of MODIS for monitoring air pollution.