Spatio-temporal variation and trends in atmospheric aerosols as well as their impact on solar radiation and clouds are crucial for regional and global climate change assessment. These topics are not so well-documented over Malaysia, the fact that it receives considerable amounts of pollutants from both local and trans-boundary sources. The present study aims to analyse the spatio-temporal evolution and decadal trend of Aerosol Optical Depth (AOD) from Terra and Aqua MODIS sensors, to identify different types and origin of aerosols and explore the link between aerosols and solar radiation. AOD and fine-mode fraction (FMF) products from MODIS, AOD and Ångström Exponent (AE) values from AERONET stations along with ground-based PM10 measurements and solar radiation recordings at selected sites in Peninsular Malaysia are used for this scope. The MODIS AODs exhibit a wide spatio-temporal variation over Peninsular Malaysia, while Aqua AOD is consistently lower than that from Terra. The AOD shows a neutral-to-declining trend during the 2000s (Terra satellite), while that from Aqua exhibits an increasing trend (~0.01 per year). AERONET AODs exhibit either insignificant diurnal variation or higher values during the afternoon, while their short-term availability does not allow for a trend analysis. Moreover, the PM10 concentrations exhibit a general increasing trend over the examined locations. The sources and destination of aerosols are identified via the HYSPLIT trajectory model, revealing that aerosols during the dry season (June to September) are mainly originated from the west and southwest (Sumatra, Indonesia), while in the wet season (November to March) they are mostly associated with the northeast monsoon winds from the southern China Sea. Different aerosol types are identified via the relationship of AOD with FMF, revealing that the urban and biomass-burning aerosols are the most abundant over the region contributing to a significant reduction (~-0.21MJm-2) of the solar radiation. © 2013 Elsevier B.V.