A chemical mass balance model developed by the U.S. EPA, CMB8.2, was used to apportion the major sources of PAHs found in the sediments of Lake Calumet and surrounding wetlands in southeast Chicago. The results indicate the feasibility of applying CMB8.2 to pollutants found in aquatic sediments. To establish the fingerprints of PAH sources, 28 source profiles were collected from the literature. Some of the source profiles were modified based on the gas/particle partitioning of individual PAHs. The profiles under the same source category were averaged, and the fingerprints of six sources were established, including coke oven, residential coal burning, coal combustion in power generation, gasoline engine exhaust, diesel engine exhaust, and traffic tunnel air. Nine model operations with a total of 422 runs were made, differing in the choice of fitting species and the sources involved. Modeling results indicate that coke ovens and traffic are the two major sources of PAHs in the area. For traffic sources, either traffic tunnel alone or both diesel and gasoline engine exhausts were entered into the model. These two groups of model operations produced comparable results with regard to the PAH contributions from road traffic. Although the steel industries have shrunk in recent years, closed and still-active coke plants continue to contribute significantly to the PAH loadings. Overall, the average contribution from coke oven emissions calculated by different operations ranges from 21% to 53% of all sources, and that from traffic ranges from 27% to 63%. The pattern of source contributions shows spatial and temporal variations.