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Currently, there is an effort under way to encourage remedial project managers at contaminated sites to use passive sampling to collect freely dissolved concentrations (C-free) of hydrophobic organic contaminants to improve site assessments. The objective of the present study was to evaluate the use of passive sampling for measuring water column C-free for several hydrophobic organic contaminants at 3 US Environmental Protection Agency Superfund sites. Sites investigated included New Bedford Harbor (New Bedford, MA, USA), Palos Verdes Shelf (Los Angeles, CA, USA), and Naval Station Newport (Newport, RI, USA); and the passive samplers evaluated were polyethylene, polydimethylsiloxane-coated solid-phase microextraction fibers, semipermeable membrane devices, and polyoxymethylene. In general, the different passive samplers demonstrated good agreement, with C-free values varying by a factor of 2 to 3. Further, at New Bedford Harbor, where conventional water sample concentrations were also measured (i.e., grab samples), passive sampler-based C-free values agreed within a factor of 2. These findings suggest that all of the samplers were experiencing and measuring similar C-free during their respective deployments. Also, at New Bedford Harbor, a strong log-linear, correlative, and predictive relationship was found between polyethylene passive sampler accumulation and lipid-normalized blue mussel bioaccumulation of polychlorinated biphenyls (r(2)=0.92, p<0.05). The present study demonstrates the utility of passive sampling for generating scientifically accurate water column C-free values, which is critical for making informed environmental management decisions at contaminated sediment sites. Environ Toxicol Chem 2015;34:1720-1733. Published 2015 SETAC. This article is a US Government work and is in the public domain in the USA.