The present study compiles new and literature data in a GIS platform aiming to (a) evaluate the extent and magnitude of Cr contamination in a Mediterranean region (Assopos-Thiva and Central Evia (Euboea) Basins, Greece); (b) combine spatial distribution of Cr in soil and groundwater with land use maps; (c) determine geochemical constraints on contamination by Cr; and (d) provide information that will be useful for better management of land use in a Mediterranean type ecosystem in order to prevent further degradation of natural resources. The spatial diversity of Cr distribution in soils and groundwater throughout the C. Evia and Assopos-Thiva Basins is considered. It is attributed to both natural Cr sources (Cr-bearing peridotites, affecting primarily soil) and human (industrial) activities (the dominant source of groundwater contamination). A combination of the spatial distribution of metals in soil and land use maps was used to define the specific areas of agricultural land use with elevated heavy metal contents. Furthermore, the combination of the spatial distribution of Cr in groundwater and land use maps allows for definition of specific areas of industrial land use with elevated Cr concentrations (Inofita, south Assopos-Thiva Basin). Despite the good correlation (r = 0.75) between Cr(VI) and the strong oxidant NO3− in C. Evia, the lower standard potential (E0) values for NO3− compared to those for Cr2O72− (the latter is a stronger oxidant than the former) suggest that NO3− is not an oxidant of Cr. This detailed assessment and presentation of the available analytical data for soil and groundwater in Assopos-Thiva and C. Evia Basins on a land use map provides information for land management decision makers.