The Thriassio plain is located 25 km west of Athens city, the capital of Greece. Two major towns (Elefsina and Aspropyrgos), heavy industry plants, medium to large-scale manufacturing, logistics plants, and agriculture comprise the main land uses of the studied area. The aim of the present study was to measure the total and available concentrations of Cr, Zn, Ni, Pb, Co, Mn, Ba, Cu, and Fe in the top soils of the plain, and to asses soil contamination by these metals by using the geoaccumulation index (I geo), the enrichment factor (EF), and the availability ratio (AR) as soil pollution indexes. Soil samples were collected from 90 sampling sites, and aqua regia and DTPA extractions were carried out to determine total and available metal forms, respectively. Median total Cr, Zn, Ni, Pb, Co, Mn, Ba, Cu, and Fe concentrations were 78, 155, 81, 112, 24, 321, 834, 38, and 16 × 10(3) mg kg(-1), respectively. The available fractions showed much lower values with medians of 0.4, 5.6, 1.7, 6.9, 0.8, 5.7, 19.8, 2.1, and 2.9 mg kg(-1). Though median total metal concentrations are not considered as particularly high, the I geo and the EF values indicate moderate to heavy soil enrichment. For certain metals such as Cr, Ni, Cu, and Ba, the different distribution patterns between the EFs and the ARs suggest different origin of the total and the available metal forms. The evaluation of the EF and AR data sets for the soils of the two towns further supports the argument that the EFs can well demonstrate the long-term history of soil pollution and that the ARs can adequately portray the recent history of soil pollution.