This study investigated the distribution features of uranium-238 (238U), radium-226 (226Ra), thorium-232 (232Th), and potassium-40 (40K) and evaluated the associated environmental radiological hazards of the topsoil and river sediments in the Jinding lead-zinc (Pb-Zn) mine catchment from Southwest China. The activity concentrations of 238U, 226Ra, 232Th, and 40K ranged from 24.0 ± 2.29–60.3 ± 5.26 Bq.kg-1, from 32.5 ± 3.95–69.8 ± 3.39 Bq.kg-1, from 15.3 ± 2.24–58.3 ± 4.92 Bq.kg-1, and from 203 ± 10.2–1140 ± 27.4 Bq.kg-1, respectively. The highest activity concentrations for all these radionuclides were primarily found in the mining areas and decreased with increasing distance from the mining sites. The radiological hazard indices, including radium equivalent activity, absorbed gamma dose rate in the air, outdoor annual effective dose equivalent, annual gonadal dose equivalent, and excess lifetime cancer, revealed that the highest values were observed in the mining area and downstream, specifically in the vicinity of the ore body. These elevated values exceeded the global mean value but remained below the threshold value, suggesting that routine protection measures for Pb-Zn miners during production activities are sufficient. The correlation analysis and cluster analysis revealed strong associations between radionuclides such as 238U, 226Ra, and 232Th, indicating a common source of these radionuclides. The activity ratios of 226Ra/238U, 226Ra/232Th, and 238U/40K varied with distance, suggesting the influence of geological processes and lithological composition on their transport and accumulation. In the mining catchment areas, the variations in these activity ratios increased indicated the impact of limestone material dilution on the levels of 232Th, 40K, and 238U in the upstream region. Moreover, the presence of sulfide minerals in the mining soils contributed to the enrichment of 226Ra and the removal of 238U caused those activity ratios decreased in the mining areas. Therefore, in the Jinding PbZn deposit, the patterns of mining activities and surface runoff processes in the catchment area favored the accumulation of 232Th and 226Ra over 40K and 238U. This study provides the first case study on the geochemical distributions of natural radionuclides in a typical Mississippi Valley-type PbZn mining area and offers fundamental information on radionuclide migration and baseline radiometric data for PbZn deposits worldwide.