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Satellite aerosol remote sensing entered a new era with the deployment of advanced satellite imaging instruments such as the Moderate Resolution Imaging Spectroradiometer (MODIS) on the NASA Terra and Aqua satellites. These new instruments provide the opportunity to learn more about aerosol properties than was possible using the simpler NOAA Advanced Very High Resolution Radiometer (AVHRR), which has been used to retrieve aerosol optical thickness for more than 20 years. Combining historical AVHRR and the more advanced MODIS aerosol retrievals to form a long-term aerosol data record is critical for studying aerosol climate forcing. To achieve this objective, it is necessary to build a connection and establish consistency between the two retrievals through a careful evaluation of the two retrieval methods applied to the same data. As a first step in this effort, this paper exploits the potential of the Clouds and the Earth’s Radiant Energy System (CERES) Single-Scanner Footprint (SSF) data set that includes aerosol products derived from Terra MODIS data at the same locations using both the multichannel MODIS and the two-channel AVHRR aerosol retrieval algorithms. The analysis examines the differences in the results seen over oceans on a global scale. It was found in a global mean sense that advancement in the aerosol retrieval over ocean from the MODIS algorithm relative to the AVHRR method is realized mostly in the improvement of the aerosol size parameter (ASP) rather than in the aerosol optical thickness (AOT). However, regional differences were observed in both AOT and ASP retrieved from the MODIS and AVHRR algorithms. These are examined further in the second part of this two-part paper. Cloud contamination and surface roughness appear to affect both aerosol retrievals, effects that need further investigation.