ABSTRACT The concentrations and fluxes of arsenic (As) and cadmium (Cd) were examined in the hydrological cycle, litterfall and soils in a maquis broadleaved evergreen forest stand in western Greece. The concentrations of the metals in the hydrological cycle ranged from 0.076 to 0.306 μg L−1 and 0.040–0.050 μg L−1 for As and Cd, respectively. It was found that the enrichment of As in the atmosphere was both due to suspended geogenic material and long range transfer, whereas for Cd the long range transfer was the predominant way for deposition. Two models were assessed to find the volumes of percolation water to compare the fluxes with the estimated ones derived from soil solution measurements. The daily deterministic forest-hydrological model (WBS3) was found to perform better than the physically based 1D semi-distributed soil-plant-atmosphere model (BROOK90). When calculating the total amounts of the heavy metals in soils, the statistical uncertainty derived from every soil layer has to be taken into account. The residence time of Cd in the forest floor (L + FH) of the soils was found 6.4 years, whereas that of As 36.3 years. This difference shows the mobility of Cd in comparison to As in the soils of the area.