Analysis of sections from dated sediment cores were used to establish geographic distributions and temporal trends of chlorinated hydrocarbon contaminant levels in sediments from natural waters of the Hudson River basin. Radiometric dating was based primarily on the depth distribution of 137(Cs) in the cores and on the occurrence of detectable levels of 7(Be) in surface sediment samples. Eighteen sampling sites included several along the main stem of the Hudson, its major tributaries, and components of the New York/New Jersey (NY/NJ) harbor complex. Drinking-water reservoirs were sampled to place upper limits on atmospheric inputs. Core sections were analyzed for polychlorinated biphenyls (PCBs), 1,1,1-trichloro-2,2-bis(p-chlorophenyl) ethane (DDT)-derived compounds, chlordane, and dioxins. Sediment concentrations of most contaminants at most sites have decreased significantly since the mid-1960s. The data provide a basinwide perspective on major point-source inputs of PCBs to the upper Hudson River and of 2,3,7,8-tetrachlorodibenzo-p-dioxin and DDT to the lower Passaic River. Evidence was found for significant but poorly characterized sources of PCBs and chlordane to the western NY/NJ harbor, and of highly chlorinated dioxins to the upstream sites on the main stem of the Hudson. The results indicate that analysis of dated sediment samples is a most effective and efficient monitoring tool for the study of large-scale geographic and temporal trends in levels of particle-associated contaminants.