In Oregon's Willamette River Basin (the Basin), health advisories currently limit consumption of fish that have accumulated methylmercury (MeHg) to levels posing a significant human health risk. These advisories created the requirement for a mercury total maximum daily load for the Basin, which required a greater understanding of the behavior, distribution, and levels of mercury and MeHg in the Basin. In 2002, the Oregon Department of Environmental Quality initiated a study to measure (using ultraclean techniques) mercury and MeHg levels in water, sediment, and fish samples collected throughout the Basin. Results from the Middle Fork (nominal background) suggested that naturally occurring surface-water concentrations of mercury and MeHg would on an annual average basis be expected in the range of 0.5 to 1.0 and 0.04 to 0.06 ng L(-1), respectively. Concentrations in the Coast Fork (Cottage Grove), which were markedly higher, are likely the result of historical mining discharges. The possibility exists that wetlands alone could contribute the dissolved MeHg levels (approximately 0.04 ng L(-1)) observed in the Main Stem. Mercury levels in sediment were similar, and near background, in the Main Stem, Coast Fork (Row River), and Middle Fork but significantly increased in the Coast Fork (Cottage Grove). Fish tissue mercury levels were typically highest in piscivorous and lowest in invertivorous species but highest in the Coast Fork (Cottage Grove). In the Coast Fork and Cottage Grove Reservoir, discharges from historical mercury mining activities appear to have significantly impacted water, sediment, and fish tissue levels; however these impacts do not appear to extend into the Main Stem. Basinwide mercury data are at present too spottily distributed to determine whether significant mercury point sources exist along the Main Stem.