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Volcanic regions are associated with increased environmental and human health risks due to elevated concentrations of potentially toxic elements (PTEs). Fogo Island, Cape Verde, experienced recent volcanic eruptions, which raised questions about local soils' potential to pose such risks. To better understand the local mineralogy and geochemistry, and environmental and probabilistic human health risks, we (i) investigate the distribution of selected PTEs in 140 soil samples covering different geologic units, (ii) determine major associations between minerals and geological units, (iii) calculate the potential ecological risk, and (iv) model human health risks based on Monte Carlo simulations. The results show that the soils overlaying the older pre-caldera units yield higher contents of secondary minerals (phyllosilicates and Fe-oxides), with relative enrichment of PTEs. The soils covering more recent units are enriched with primary minerals (feldspar and pyroxene) and show elevated concentrations of Pb. This study suggests that As, Pb, Cd and Hg pose ‘considerable’ to ‘very high’ ecological risks. Based on probabilistic health risk simulation, ingestion is identified as the dominant pathway of PTEs exposure. Metal(oid)s are unlikely to cause a non-carcinogenic health risk, although As may pose a cancer risk for children. This research also provides health and environmental authorities with a tool to manage such risks.