This study analyses the trends of total aerosol and the main aerosol species over nine capitals in the Baltic Sea basin from 1989 to 2019 based on the Modern-Era Retrospective Analysis for Research and Applications, Version 2 Reanalysis. Aerosol speciation includes mineral dust, sea salt, sulphate (SO4), organic carbon (OC), and black carbon (BC). The mean total aerosol optical depth (AOD) values were the highest (up to 0.216) over the continental capitals (i.e., Warsaw, Berlin, and Vilnius). For each capital, the mean SO4 AOD was the main aerosol species, with a trend specular to total AOD. Apart from Warsaw, the mean BC AOD was the aerosol species with the lowest level. The composition of aerosols changed with respect to the species of anthropogenic origins (i.e., SO4, OC, and BC), with the percentage contribution to the total AOD decreasing for the SO4 AOD and increasing for the BC AOD. Also, the OC AOD showed an increase in the percentage contribution to total AOD for Copenhagen, Oslo, Stockholm, and the continental capitals. Anthropogenic aerosols contributed up to 90.3% of the total AOD, with the highest values over the continental capitals. For each capital, the minimum in the percentage contribution of anthropogenic AOD was between 2007 and 2008, likely due to the global financial crisis. Anthropogenic AOD as a percentage of the total AOD decreased from 1989 to 2008. Both the total and the SO4 AODs decreased over each capital. By contrast, the BC AOD increased over Stockholm, and both the OC and BC AODs increased over Berlin, Copenhagen, and Oslo. The decoupling of carbonaceous aerosols and the SO4 AOD trends was likely due to concurrent factors such as biomass burning and low-sulphur fuel policies. From 2000 to 2019, the inverse relationships between gross domestic products and SO4 AODs suggest a relative decoupling of economic growth from fossil fuels for Oslo, Stockholm, Tallinn, and Vilnius.