The operational atmospheric correction algorithm for Sea-Viewing Wide Field-of-View Sensor (SeaWiFS) and Moderate Resolution Imaging Spectroradiometer (MODIS) uses the predefined aerosol models to retrieve aerosol optical properties, and their accuracy depends on how well the aerosol models can represent the real aerosol optical properties. In this paper, we developed a method to evaluate the aerosol models (combined with the model selection methodology) by simulating the aerosol retrieval using the Aerosol Robotic Network (AERONET) data. Our method can evaluate the ability of aerosol models themselves, independent of the sensor performance. Two types of aerosol models for SeaWiFS and MODIS operational atmospheric correction algorithms are evaluated over global open oceans, namely the GW1994 models and Ahmad2010 models. The results show that GW1994 models significantly overestimate the aerosol optical thicknesses and underestimate the Ångström exponent, which is caused by the underestimation of the scattering phase function. However, Ahmad2010 models can significantly reduce the overestimation of the aerosol optical thickness and the underestimation of the Ångström exponent as a whole, but this improvement depends on the backscattering angle. Ahmad2010 models have a significant improvement in the retrieval of the aerosol optical thickness at a backscattering angle less than 140°. For a backscattering angle larger than 140°, GW1994 models are better at retrieving the aerosol optical thickness than the Ahmad2010 models.