New insights about the geochemical behavior of actinides and lanthanides in an old uranium mine are provided for the first time in this work. Fifteen samples (water, soil, and sediments) were collected inside and outside the Quinta do Bispo old mine (Portugal) in order to better understand the lanthanide and actinide behavior in the soil–water system. The chemical and mineralogical composition was obtained via ICP-MS, INAA, and XRD. The water sample from the open pit exhibits a higher U and REE dissolved concentration when compared to the other water samples. A positive Eu anomaly is found in this sample. The soil samples collected inside the mine area, including mine waste rocks and the minesoils surrounding the open pit, show uranium mineral phases, higher U contents, an enrichment of LREE relative to HREE, and a lower Th/U. This heterogeneity may be due to the open pit extraction and ore processes, as well as the percolation and water infiltration through the waste rock piles. Soils from outside the mine area have a similar mineralogical and chemical composition, despite their different geological context, which could be related to the influence of the granitic geological unit during the alluvial unit deposition. The sediments have similar REE patterns, negative Eu anomaly, and a high (La/Yb)N.