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The Picoto mining area is in the village of Vilar Seco (Viseu), central Portugal. Mineralization occurs mainly in quartz veins with meta-torbernite and uranophane and some U-bearing minerals, cutting a Variscan granite. Exploitation took place in two phases, between 1917 and 1953, and since the closure, the area has never been remediated. Water–rock interaction processes, including the mobility of potentially toxic elements through soil and water (surface and groundwater), were identified with the determination in situ of physicochemical parameters and selected anions and cations, by ICP-OES. The soils are contaminated with As (>44 mg/kg), Cu (>23 mg/kg), and U (>40 mg/kg) and cannot be used for agricultural or domestic purposes. The waters are generally weakly mineralized and have pH values ranging from acidic to neutral. However, some of them are contaminated with NO2 (up to 2.3 mg/L), Fe (up to 1849 mg/L), Mn (up to 777 mg/L), Cu (up to 5.4 g/L), As (up to 14.7 g/L), and U (up to 66.2 g/L) and cannot be used for human consumption or agricultural activities. The soil and water contamination are mainly related to the old mine activities and the subsequent human activities that have developed in the area.