Waste dumps resulting from metal exploitation create serious environmental damage, providing soil and water degradation over long distances. Phytostabilization can be used to remediate these mining sites. The present study aims to evaluate the behavior of selected plant species (Erica arborea, Ulex europaeus, Agrostis delicatula, and Cytisus multiflorus) that grow spontaneously in three sulfide-rich waste-dumps (Lapa Grande, Cerdeirinha, and Penedono, Portugal). These sites represent different geological, climatic and floristic settings. The results indicate distinctive levels and types of metal contamination: Penedono presents highest sulfate and metal contents, especially As, with low levels of Fe. In contrast, at Lapa Grande and Cerdeirinha Fe, Mn, and Zn are the dominant metals. In accordance, each waste dump develops a typical plant community, providing a specific vegetation inventory. At Penedono, Agrostis delicatula accumulates As, Pb, Cu, Mn, and Zn, showing higher bioaccumulation factors (BF) for Mn (32.1) and As (24.4). At Cerdeirinha, Ulex europaeus has the highest BF for Pb (984), while at Lapa Grande, Erica arborea presents high BF for Mn (9.8) and Pb (8.1). Regarding TF, low values were obtained for most of the metals, especially As (TF < 1). Therefore, the results obtained from representative plant species suggest appropriate behavior for phytostabilization measures.