We studied the chemical composition of As and Pb in total (<2 mm) and fine fractions (<50 μm) of 52 urban soil samples from Minas de Riotinto (mining area) and Aracena (non-exposed area) in SW Spain. In addition to a soil phytotoxicity bioassay using Lactuca Sativa L., we modelled and performed carcinogenic and non-carcinogenic human health risk assessment, later comparing our data with relative cancer mortality rates reported at the municipal level. This study demonstrates that mineralized bedrock and natural soil-forming processes affect the geochemistry of natural (in-situ) urban soils, which in many cases surpass the regulatory levels for As (36 mg/kg) and Pb (275 mg/kg). Fine fractions of in-situ and mixed urban soils -susceptible of inhalation- are significantly enriched in As and Pb with respect to fine fractions of aggregate materials (ex-situ soils of chalky sands and gravel) in Minas de Riotinto. The soils in Minas de Riotinto are significantly enriched in As (total and fine fractions) and Pb (total fraction) with respect to Aracena. Despite elevated bulk concentrations of As and Pb, only one in-situ sample exhibits phytotoxic effects of the soil-water extracts on Lactuca Sativa L. seeds. Health risk assessment of these towns as exposure areas indicates that the soils of Minas de Riotinto are indeed a health risk to the residents, whereas there is no potential risk in Aracena. The reported relative mortality rates in Minas de Riotinto show a greater mortality of carcinogenic tumors potentially related to As and Pb exposure, including lung cancer. Both soil type and use must be considered when administrators or policy-makers evaluate health risks involved in urbanistic decision-making. To minimize exposure risk and adverse health outcomes, we recommend that in-situ soils surpassing regulatory levels for As and Pb in public playgrounds and passing areas should be covered with aggregate materials.