The current study was conducted to assess the level and spatial distribution of metal pollution in surface water, soil, and sediment samples from the Arieș River basin, located in central Romania, an area impacted by various mining and industrial operations. Several pollution indices, spatial distributions, cluster analyses, principal component analyses, and heat maps were applied for evaluating the contamination level with Ni, Cu, Zn, Cd, Pb, Mn, As, and Hg in the area. Based on the results of the Heavy-Metal Pollution Index and of the Heavy-Metal Evaluation Index of the surface-water samples, the middle part of the Arieș River basin, near and downstream of the gold mine impoundment, was characterized by high pollution levels. The metal concentration was higher near the tailing impoundment, with increased levels of Cu, Ni, Zn, and Pb in the soil samples and As, Cd, Pb, Na, K, Ca, Mn, and Al in the sediment samples. Ca (23.7–219 mg/L), Mg (2.55–18.30 mg/L), K (0.64–14.70 mg/L), Al (0.06–22.80 mg/L), and Mn (0.03–22.40 mg/L) had the most remarkable spatial variation among the surface-water samples, while various metal contents fluctuated strongly among the sampling locations. Al varied from 743 to 19,8 mg/kg, Fe from 529 to 11,4 mg/kg, Ca from 2316 to 11,8 mg/kg, and Mg from 967 to 2547 mg/kg in the soil samples, and Al varied from 3106 to 8022 mg/kg, Fe from 314 to 5982 mg/kg, Ca from 1367 to 8308 mg/kg, and Mg from 412 to 1913 mg/kg in the sediment samples. The Potential Ecological Risk Index values for soil and sediments were in the orders Cu > Ni > Pb > Hg > Cr > As > Mn > Zn > Cd and As > Cu > Cr > Cd > Pb > Ni > Hg > Mn > Zn, respectively, and the highest values were found around the gold mine impoundment.