The objective of this study was to determine the levels of major phytotoxic metals--including cadmium (Cd), copper (Cu), nickel (Ni), and zinc (Zn)--in agricultural soils of Western Macedonia, Greece. We also wanted to determine the possible relationships among elements and between soil properties and elemental concentrations. Surface soil samples, n = 570, were collected and analyzed. The results of the elemental analysis showed that the mean metal concentrations were consistent with reported typical concentrations found in Greek agricultural soils in the cases of Zn and Cu. Cd exhibited lower and Ni higher mean concentrations than the typical levels reported in the literature. Metal concentrations in the majority of the examined samples (>69%) were found to be higher than the respective critical plant-deficiency levels. However, only 0.4% and 0.2% of the analyzed soil samples, respectively, exhibited Cd and Ni concentrations higher than the levels that cause plant toxicity, as referenced by other investigators. These results suggest that the soils studied can be considered as unpolluted with respect to the examined food-chain metal contaminants. However, the levels of the metal concentrations in some of the soil samples, and the low correlation of the metals with soil properties, suggest an anthropogenic rather that lithogenic origin.