The assessment of potential radiation hazards in accumulated sediments in aquatic ecosystems is vital for the management and disposal of sediments. Furthermore, preemptive management of radionuclides in terrestrial ecosystems is critical for marine ecosystem conservation. We analyzed the activity concentrations of natural radionuclides (226Ra,232Th, 238U, and 40K) in the surface sediments of major river watersheds in Korea and evaluated the radiation hazards stemming from these activity concentrations. The mean activity concentrations of 226Ra and 238U were lower than the global average, whereas those of 232Th and 40K were higher. The mean values of radium equivalent activity, external hazard index, and internal hazard index calculated from these activity concentrations did not exceed the recommended maximum values. The mean values of absorbed gamma dose rate in air and annual outdoor effective dose rate (AEDRout) were higher than the global average by the United Nations Scientific Committee on the Effects of Atomic Radiation (UNSCEAR) but remarkably lower than the recommended and background values by the International Commission on Radiological Protection (ICRP) and the Korea Institute of Nuclear Safety (KINS). The contribution of 40K and 232Th to the AEDRout mean value was predominant. In conclusion, the surface sediments of major river watersheds in Korea are associated with negligible radiation hazards. These findings provide fundamental data for the management and treatment of sediments in terrestrial and marine ecosystems.