The present study analyzes PM(10) concentration data collected by the Greek air quality monitoring network at 8 sites over the Greater Athens Area, for the period of 2001-2004. The primary objectives were to assess the degree of compliance with the EU-legislated air quality standard for PM(10) and also provide an overall statistical examination of the factors controlling the seasonal and spatial variation of concentrations, over the wider urban agglomeration. Daily concentrations, averaged over the whole study period, ranged between 32.3 and 60.9 microg m(-3). The four-year average concentration of PM(10) at five sites exceeded the annual limit value of 40 microg m(-3), while most of the sites surpassed the allowed percentage of exceedances of the daily limit value (50 microg m(-3)), for each of the four years. The seasonal variation of PM(10) levels was not found to be uniform across the eight sites, with average cold-period concentrations being higher at four of them and warm period concentrations being significantly higher at three sites, which also displayed recurring annual variation of monthly concentrations. Concentration levels displayed moderate spatial heterogeneity. Nevertheless significant inter-site correlations were observed (ranging between 0.55 and 085). The determination of the spatial correlation levels relied mainly on site types rather than on inter-site distances. Monitoring sites were classified accordingly using cluster analysis in two groups presenting distinct spatiotemporal variation and affected by different particle formation processes. The group including urban sites was mainly affected by primary, combustion-related processes and especially vehicular traffic, as it was also deduced through the examination of the diurnal distribution of particulate levels and through factor analysis. On the contrary, suburban background sites seemed more affected by particle transport from more polluted neighboring areas and secondary particle formation through gaseous precursors, both processes aided from favoring meteorological conditions. The association of the PM(10) levels with backwards trajectories was also examined, in an attempt to account for the possible long range transport of particles in Athens. It was found that a notable part of area-wide episodic events could be attributed to trans-boundary transport of particles, with the origins of some severe dust outbreaks traced back to the Sahara desert and the Western Mediterranean.