The Ife-Ilesha schist belt in southwest Nigeria is one of the most mineralized schist belts in Nigeria. Large amount of wastes are generated during mining processes and accumulate as tailings within the mining environment. These tailings, which contain high concentrations of natural radionuclides and potentially toxic elements, are washed into mining ponds in the mining environment. The water in these mining ponds is utilized by miners and populations around the mining sites, thereby causing serious negative health effects on humans and the environment. Water samples were collected from mining pits and waste water ponds in five gold mining sites and a kaolin mining site within the Ife-Ilesha schist belt. Activity concentrations of natural radionuclides (⁴⁰K, ²³⁸U, and ²³²Th) and potential toxic elements (PTEs) have been measured using gamma and atomic absorption spectroscopies. The results show that average concentrations of ⁴⁰K, ²³⁸U, and ²³²Th in the mine waters are 217 ± 40, 10 ± 09 and 16 ± 02 Bq/kg, which are far higher than their permissible level in water. The average concentrations PTEs decrease according to the sequence; Zn > Cr > Cu > Pb > As > Cd > Ni. The concentrations of As, Cd and Cr, exceeded their respective limits in mine water. Based on the results of this research, it can be concluded that the mine waters pose significant radiological risks. The results of PTEs show potential risks to both humans and the environment from the mine waters.