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Spatial patterns of bioaccumulated mercury were evaluated in coastal marine food webs of east Hudson Bay and east James Bay in the boreal subarctic of Canada. Two marine species, blue mussels (Mytilus edulis) and common eider ducks (Somateria mollissima) that consume mussels, were collected by a regional community-based monitoring network established in five communities. Stable isotope tracers (carbon, nitrogen, sulfur, and mercury) were measured to evaluate environmental drivers of mercury spatial patterns. Mercury concentrations of blue mussels and common eiders were twofold and fivefold higher, respectively, on the James Bay coast near the community of Chisasibi compared to sites in east Hudson Bay. Liver and muscle mercury concentrations of eiders from James Bay are among the highest values reported for the circumpolar subarctic and Arctic. Multiple lines of evidence (mercury spatial patterns, crustal elements in blue mussels, and mercury isotope values of common eiders) suggest elevated mercury in the coastal food web of east James Bay may be due to mercury loading from the La Grande River, which drains one of the largest hydroelectric developments in the world. These findings highlight the importance of further research on environmental processes linking large rivers to mercury bioaccumulation in northern coastal food webs.