The closure of mercury mining areas is generally associated with a release of Hg and other metals into the environment due to the abandonment of mining wastes. Because of their potential toxic properties, the mobilization of particulate and soluble metal species is of major concern. In the present study, the environmental risks posed by soils surrounding an abandoned mercury mining area in Valle del Azogue (Almeria, Spain) are assessed through the determination of physical-chemical parameters, the quantification of metal concentrations, and the application of aquatic and terrestrial ecotoxicity bioassays. Chemical analysis of soil samples revealed concentrations of Hg, As, Ba, Pb, Sb, and Zn above international intervention values. Results from terrestrial tests showed detrimental effects in all studied organisms (Eisenia foetida, Folsomia candida, and different plant species) and revealed the avoidance response of earthworms as the most sensitive endpoint. Surprisingly, the most toxic samples were not the ones with higher metal contents but the ones presenting higher electrical conductivity. Aquatic ecotoxicity tests with Vibrio fischeri, Raphidocelis subcapitata, Daphnia magna, and Danio rerio were in accordance with terrestrial tests, confirming the need to couple environmental chemistry with ecotoxicological tools for the proper assessment of metal-contaminated sites. In view of the results, a remediative intervention of the studied area is recommended