The Itakpe abandoned iron-ore mines constitute the largest iron-ore deposits in Nigeria with an estimated reserve of about three million metric tons of ore. The present effort is a part of a comprehensive study to estimate the environmental and radiological health hazards associated with previous mining operations in the study area. In this regard, heavy metals (Fe, Zn, Cu, Cd, Cr, Mn, Pb, Ni, Co and As) and natural radionuclides (U, Th and K) were measured in rock, soil and water samples collected at different locations within the mining sites. Atomic absorption and gamma-ray spectrometry were utilized for the measurements. Fe, Mn, Zn, Cu, Ni, Cd, Cr, Co Pb and As were detected at varying concentrations in rock and soil samples. Cd, Cr, Pb and As were not detected in water samples. The concentrations of heavy metals vary according to the following pattern; rock ˃ soil ˃ water. The mean elemental concentrations of K, U and Th are 2.9%, 0.8 and 1.2 ppm and 1.3%, 0.7 and 1.7 ppm, respectively, for rock and soil samples. Pearson correlation analyses of the results indicate that the heavy metals are mostly negatively correlated with natural radionuclides in the study area. Cancer and non-cancer risks due to heavy metals and radiological hazards due to natural radionuclides to the population living within the vicinity of the abandoned mines are lower than acceptable limits. It can, therefore, be concluded that no significant environmental or radiological health hazard is envisaged.