Aerosol Optical Depth (AOD) measurements from Aerosol Robotic NETwork (AERONET; level 2.0), Microtops - II sun-photometer and MODerate Resolution Imaging Spectroradiometer (MODIS) (Terra and Aqua; level 2, collection 5, dark target) were compared and used to characterize aerosols over Pune, India. AODs from Microtops and MODIS were compared with those measured by AERONET to evaluate the measurement quality. To the best of our knowledge, this is the first systematic comparison of MODIS aerosol products over Pune, India. The results of the analysis show that during 2008–10, 68% to 84% of the MODIS AODs fell within an expected error, as defined by the MODIS science team, and thus the retrievals from this system are validated and accepted. In addition, during pre-monsoon periods MODIS retrievals are better-matched with ground-based measurements. On the seasonal scale, MODIS retrievals corroborate well with ground-based measurements, with correlation coefficients ranging from 0.62 to 0.93. Despite an overall satellite-ground agreement, MODIS tends to under-estimate AOD during winter, and this may be due to improper assumptions of surface reflectance and the incorrect selection of aerosol types. AERONET retrieved single scattering albedo (SSA) values in winter (0.82–0.86), suggesting the dominance of absorbing aerosols, slightly increased (0.87–0.89) in pre-monsoon season, indicating more scattering type of aerosols. These values are about 8.9%–1.1% lower than those of the assumed SSA values in the MODIS algorithm.