From 1990 to 1994, a total of 21 sediment cores and 37 grab sediment samples were collected from the Milwaukee Harbor Estuary. Each sediment core was sectioned and dated using ²¹⁰Pb and¹³⁷ Cs radioisotope techniques. A total of 305 samples were analyzed for sixteen polycyclic aromatic compounds (PAHs). Grain size distribution, porosity, and total organic carbon content as measured by loss on ignition were also determined. The results provide a historical overview of the impact of industrialization in the Milwaukee area. Although highly variable, the concentration profile of PAHs show, in general, peaks in the 1950's through 1980's. The PAH concentrations have declined since then for most sediment cores. The current levels of total PAHs in most surface sediment samples range from 25 to 200 ppm. A few cores, some of which were collected in 1994, have an elevated PAH concentration at the surface. Toxicity of the surface sediments was evaluated by comparing with the benchmark values developed by the United States National Oceanic and Atmospheric Administration (NOAA). The most heavily contaminated area was found in the Kinnickinnic River between the Becher Street Bridge and the Wisconsin Wrecking Company Wharf. The highest total PAH concentration determined from seven vibra cores collected in this area ranges from 380 to 1000 ppm. The former Wisconsin Solvay Coke Company may have been a major point source of PAHs until the 1970's. Highway traffic and various industrial discharges also contribute to the sediment PAHs in this area.