Trophic transfer of perfluorooctanesulfonate (PFOS) and other related perfluorinated compounds was examined in a Great Lakes benthic foodweb including water-algae-zebra mussel-round goby-smallmouth bass. In addition, perfluorinated compounds were measured in livers and eggs of Chinook salmon and lake whitefish, in muscle tissue of carp, and in eggs of brown trout collected from Michigan. Similarly, green frog livers, snapping turtle plasma, mink livers, and bald eagle tissues were analyzed to determine concentrations in higher trophic-level organisms in the food chain. PFOS was the most widely detected compound in benthic organisms at various trophic levels. Concentrations of PFOS in benthic invertebrates such as amphipods and zebra mussels were approximately 1000-fold greater than those in surrounding water, which suggested a bioconcentration factor (BCF; concentration in biota/concentration in water) of 1000 in benthic invertebrates. Concentrations of PFOS in round gobies were two- to fourfold greater than those in their prey organisms such as zebra mussels and amphipods. Concentrations of PFOS in predatory fishes (Chinook salmon and lake whitefish) were 10 to 20-fold greater than those in their prey species. Concentrations of PFOS in mink and bald eagles were, on average, 5- to 10-fold greater than those in Chinook salmon, carp, or snapping turtles. Because of the accumulation of PFOS in liver and blood, the biomagnification factor (BMF) of perfluorinated compounds in higher trophic-level organisms such as salmonid fishes, mink, and eagles were based on the concentrations in livers or plasma. Overall, these results suggest a BCF of PFOS of approximately 1000 (whole-body based) in benthic invertebrates, and a BMF of 10 to 20 in mink or bald eagles, relative to their prey items. Eggs of fish contained notable concentrations of PFOS, suggesting oviparous transfer of this compound. PFOA was found in water, but its biomagnification potential was lower than that of PFOS.