The radioactivity associated with artisanal and small-scale gold mining activities (ASM) carried out along the Ulindi River, in the eastern Democratic Republic of the Congo, was evaluated by gamma-ray spectrometry and inductively coupled plasma–mass spectrometry of soil and sediment samples. The results revealed that activity concentrations of 238U (up to 3127 ± 98 Bq kg−1), 226Ra (up to 2710 ± 89 Bq kg−1) and 232Th (up to 2142 ± 162 Bq kg−1) were 71- to 89-fold higher than the worldwide average concentrations reported by UNSCEAR in soils. Primordial radionuclides are, thus, present in high concentrations in deposits of gold in that region and the average ambient effective radiation dose rate was determined at 8.4 mSv y−1 (range 0.5 to 40 mSv y−1). This area may be classified as a natural high background radiation area (HBRA). The radiation risk for artisanal miners and population members manipulating those geological materials were assessed through radiological parameters. such as the radium equivalent activity index (RaEq), outdoor gamma absorbed dose rate (ODRA), annual effective dose equivalent (AEDE), and excess lifetime cancer risk (ELCR). The mean values of these parameters were significantly elevated in comparison to the world average levels and indicated the existence of significant radiation risks for gold miners and members of the local population. A radiation safety policy seems needed to protect workers and the local population in this region.