Concentration of aliphatic, aromatic, and chlorinated hydrocarbons were determined from 33 surface-sediment samples taken from the Tidal Basin, Washington Ship Channel, and the Anacostia and Potomac rivers in Washington, D.C. In conjunction with these samples, selected storm sewers and outfalls also were sampled to help elucidate general sources of contamination to the area. All of the sediments contained detectable concentrations of aliphatic and aromatic hydrocarbons, DDT (total dichlorodiphenyltrichloroethane), DDE (dichlorodiphenyldichloroethene), DDD (dichlorodiphenyldichloroethane), PCBs (total polychlorinated biphenyls) and total chlordanes (oxy-, α-, and γ-chlordane and cis + trans-nonachlor). Sediment concentrations of most contaminants were highest in the Anacostia River just downstream of the Washington Navy Yard, except for total chlordane, which appeared to have upstream sources in addition to storm and combined sewer runoff. This area has the highest number of storm and combined sewer outfalls in the river. Potomac River stations had lower concentrations than other stations. Total hydrocarbons (THC), normalized to the fine-grain fraction (clay + silt, < 63 μm), ranged from 120 μg g−1 to, 1,900 μg g−1 fine-grain sediment. The hydrocarbons were dominated by the unresolved complex mixture (UCM), with total polycyclic aromatic hydrocarbons (PAHs) concentrations ranging from 4 μg g−1 to 33 μg g−1 fine-grain sediment. Alkyl-substituted compounds (e.g., C1 to C4 methyl groups) of naphthalene, fluorene, phenanthrere + anthracene, and chrysene series dominated the polycyclic aromatic hydrocarbons (PAHs). Polycyclic aromatic hydrocarbons, saturated hydrocarbons, and the unresolved complex mixture (UCM) distributions reflect mixtures of combustion products (i.e., pyrogenic sources) and direct discharges of petroleum products. Total PCB concentrations ranged from 0.075 μg g−1 to 2.6 μg g−1 fine-grain sediment, with highest concentrations in the Anacostia River. Four to six C1-substituted biphenyls were the most-prevalent PCBs. Variability in the PCB distribution was observed in different sampling areas, reflecting, differing proportion of Arochlor inputs and degradation. The concentration of all contaminants was generally higher in sediments closer to known sewer outfalls, with concentrations of total hydrocarbon, PAHs, and PCBs as high as 6,900 μg g−1, 620 μg g−1, and 20 μg g−1 fine-grain sediment, respectively. Highest PCB concentrations were found in two outfalls that drain into the Tidal Basin. Concentrations of organic contaminants from sewers draining to the Washington Ship Channel and Anacostia River had higher concentrations than sediments of the mid-channel or river. Sources of PCBs appear to be related to specific outfalls, while hydrocarbon inputs, especially PAHs, are diffuse, and may be related to street runoff. Whereas most point-source contaninant inputs have been regulated, the importance of nonpoint source inputs must be assessed for their potential addition of contaminants to aquatic ecosystems. This study indicates that in large urban areas, nonpoint sources deliver substantial amounts of contaminants to ecosystems through storm and combined sewer systems, and control of these inputs must be addressed.