[abstract] A negative trend is being revealed in the MODIS aerosol optical depth [AOD] observed over the Southern Balkan/Eastern Mediterranean region. Collection 005 MODIS/Terra and MODIS/Aqua AOD at 470 nm measurements were evaluated against Brewer ground-based measurements over Thessaloniki, Greece and CIMEL ground-based measurements of AOD over Heraklion, Crete. A detailed study of the monthly, seasonal and inter-annual variability of the MODIS/Terra and MODIS/Aqua AOD values over selected locations around the Balkan Peninsula showed that the higher mean AOD values occurred in the spring and summer months, whereas the lowest were found in the winter-time. For all seasons, the highest AODs were observed for the northern-most latitudes with a marked decrease towards the southern-most sites. A statistically significant decreasing trend in aerosol load in the region over all sites as derived from the MODIS/Terra measurements gave the highest per annum change seen for the summer months to be -4.09 ± 2.34%, and the lowest for the winter months as -2.55 ± 4.36%, which also shows the higher variability.