The study objective was to determine whether environmental radionuclide accumulations were occurring in an aquatic system with a 13-y history of supplying a power plant with reactor-cooling water as well as receiving plant discharge. The aquatic system consisted of the following: 1) a reactor-cooling lake; 2) a secondary lake approximately 8 km downstream; and 3) a small stream that interfaced with the two lakes. Gamma-emitting radionuclides were identified and quantified in samples of benthic sediments obtained from representative areas of the aquatic system. This study demonstrated that in a reactor-aquatic cooling system, the component of the aquatic system most likely to experience radionuclide accumulation will not necessarily be the reactor-cooling lake, but will be that component of the aquatic system whose benthic sediments contain the highest concentrations of organic matter. Further, it was shown that the quantity of oxidizable organic matter present in a sediment is a good predictor or marker for potential sites of radionuclide accumulation (i.e., 60Co and 137Cs).