An abandoned sphalerite mining area in the southwest (SW) of the Iberian Peninsula was studied to evaluate the impact that the presence of metal(loid)s has on soil and ecosystem health. Five zones were delimited: sludge, dump, scrubland, riparian zone, and dehesa. Critical total levels of lead (Pb), zinc (Zn), thallium (Tl), and chromium (Cr), well above the limit indicative of toxicity problems, were found in the areas close to the sources of contamination. Pb-Zn concentrations were very high in the riparian zone, reaching values of 5875 mg/kg Pb and 4570 mg/kg Zn. The whole area is classifiable as extremely contaminated with Tl, with concentrations above 370 mg/kg in the scrubland. Cr accumulation mainly occurred in areas away from the dump, with levels up to 240 mg/kg in the dehesa. In the study area, several plants were found growing luxuriantly despite the contamination. The measured metal(loid)s content is the cause of a significant decrease in ecosystem services, resulting in unsafe soils for food and water production, so the implementation of a decontamination program is advisable. The plant species Retama sphaerocarpa, present in the sludge, scrubland, riparian zone, and dehesa, is postulated as suitable for use in phytoremediation.