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Review of data from several contaminated sediment sites suggested that biota-sediment accumulation factors (BSAFs) declined with increasing contaminant concentrations in the sediment. To evaluate the consistency and possible causes of this behavior, polychlorinated biphenyl (PCB)-contaminated sediment samples from the Hudson, Grasse, and Fox River Superfund sites were used in sediment bioaccumulation tests with the freshwater oligochaete, Lumbriculus variegatus, with PCB concentrations in interstitial water (IW) quantified using polyoxymethylene passive samplers. Measured BSAFs tended to decrease with increasing PCB concentration in sediment, especially for the more highly chlorinated congeners. Measures of partitioning between sediment, IW, and oligochaetes showed that measured sediment-IW partition coefficients (KTOC) tended to increase slightly with increasing sediment contamination, whereas the ratio of tissue PCB to IW PCB tended to decrease with increasing concentration in IW. Variation in accumulation among sediments was clearly influenced by bioavailability, as reflected by IW measurements, although the specific cause of varying KTOC was not clear. Calculated partitioning between IW and organism lipid (Klipid) indicated that accumulation was generally 5 to 10-fold higher than would be predicted if Klipid was approximately equal to the n-octanol-water partition coefficient (KOW). While affirming previous observations of decreasing BSAFs with increasing PCB contamination, the relatively shallow slope of the observed relationship in the current data may suggest that this concentration dependence is not a major uncertainty in sediment risk assessment, particularly if measurements of PCBs in IW are incorporated. Environ Toxicol Chem 2013;32:1495-1503. (c) 2013 SETAC