In Berlin, NH, the Androscoggin River flows adjacent to a former chlor-alkali facility that is a US EPA Superfund site and source of mercury (Hg) to the river. A study was conducted to determine the fate and bioaccumulation of methylmercury (MeHg) to lower trophic-level taxa in the river. Surface sediment directly adjacent to the source showed significantly elevated MeHg (10–40x increase, mean±sd: 20.1±24.8 ng g−1 DW) and total mercury (THg, 10–30x increase, mean±sd: 2045±2669 ng g−1 DW) compared to all other reaches, with sediment THg and MeHg from downstream reaches elevated (3–7x on average) relative to the reference (THg mean±sd: 33.5±9.33 ng g−1 DW; MeHg mean±sd: 0.52±0.21 ng g−1 DW). Water column THg concentrations adjacent to the point source for both particulate (0.23 ng L−1) and dissolved (0.76 ng L−1) fractions were 5-fold higher than at the reference sites, and 2–5-fold higher than downstream. Methylmercury production potential (MPP) of periphyton material was highest (2–9 ng g−1 d−1 DW) adjacent to the Superfund site; other reaches were close to or below reporting limits (0. 1 ng g−1 d−1 DW). Total Hg and MeHg bioaccumulation in fauna was variable across sites and taxa, with no clear spatial patterns downstream of the contamination source. Crayfish, mayflies and shiners showed a weak positive relationship with porewater MeHg concentration.