Abandoned mining areas provide valuable opportunities to investigate ore-forming processes, supergene mineral transformations, and the geochemical behaviour of metals. In this sense, the old Preguiça mine (Beja, Portugal), exploited for Fe–Zn–Pb, was studied providing new mineralogical and geochemical data aimed at improving the understanding of the secondary mineral assemblages of this deposit. A total of 70 samples collected from three accessible underground levels (first, second and third) and mine waste, complemented by 16 samples from a deeper level (fourth) previously collected, were analysed using X-ray diffraction (XRD), scanning electron microscopy (SEM), and a portable X-ray fluorescence (pXRF) equipment. Mineralogical phases are dominated by a wide range of secondary oxides, carbonates, arsenates, vanadates, silicates, phosphates and sulphates, but remnants of primary sulphides were also found. The following minerals can be emphasised: goethite, hematite, calcite, dolomite, descloizite, willemite, mimetite, cerussite, smithsonite and fraipontite. The presence of massicot in the Preguiça mine, is described for the first time. Bulk geochemical analyses show high concentrations of Fe, Ca, Zn and Pb, consistent with the observed mineralogy. The presence of vanadium- and arsenic-bearing minerals highlights the occurrence of critical raw materials, supporting the importance of reassessing other abandoned mining areas in the context of sustainable resource management and strategic raw-material planning.