This study presents an overview about the arsenic (As) contamination and its sources in two European countries. Arsenic is a highly toxic element in its inorganic form and it is carcinogenic to human seven in low concentrations. The occurrence of As in surface water, stream and marine waters, groundwater, bottled water, sediment, soil, mines, and seafood, its environmental origin, and its impacts on human health are discussed. The classes of Geoaccumulation Index for As in Greece ranges from practically uncontaminated to extremely contaminated, and in Cyprus varies between practically uncontaminated and heavily contaminated. In many cases, the As contamination reaches very high concentrations and the impacts may be crucial for the human health and ecosystems. Physicochemical properties, regional climate and geological setting are controlling the occurrence and transport of As. In Greece and Cyprus, the geology, lithology, and ore-deposits are the most important factors for the variation of As contents in water, soil, and sediment. The dominant As species are also determined by the location and the redox conditions. The findings of this paper may be useful for scientists and stakeholders monitoring the studied areas and applying measures for protection of the human and terrestrial ecological receptors (plants, avian, mammals).