The main uncertainties regarding the estimation of changes in the Earth’s energy budget are related to the role of atmospheric aerosols. These changes are caused by aerosol–radiation and aerosol–cloud interactions, which heavily depend on aerosol properties. Since the 1980s, many international modelling initiatives have studied atmospheric aerosols and their climate effects. This work carried out under the AQMEII3 initiative, in collaboration with the HTAP2 action, aims to evaluate the representativeness of Aerosol Optical Depth (AOD) and the Ångström coefficient over the entire European domain. The evaluation was made using remote-sensing data from the Moderate Resolution Imaging Spectroradiometer (MODIS) sensors aboard the Terra and Aqua platforms. The results showed the ability of the simulations performed in reconstructing the AOD, especially the more average and low values (below 0.5), while the higher values (close to 1) are either underestimated (events characterised by strong emissions from biomass burning) or overestimated (events characterised by strong dust contributions from desert areas). In contrast, the spatial and temporal distribution of AOD is generally well reproduced by all models. The Ångström coefficient showed more significant errors, with strong underestimation of spatial variability by all models.