Deposition of inorganic mercury (Hg) from the atmosphere remains the principle source of Hg contamination for most aquatic ecosystems. Inorganic Hg is readily converted to toxic methylmercury (MeHg) that bioaccumulates in aquatic food webs and may pose a risk to piscivorous fish and wildlife. We conducted a screening-level risk assessment to evaluate the extent of risk to top aquatic piscivores: the common loon (Gavia immer), walleye (Sander vitreus), and northern pike (Esox lucius). Risk quotients (RQs) were calculated on the basis of a dietary Hg exposure indicator (HgPREY) modeled from over 230,000 observations of fish Hg concentrations at over 1900 locations across Canada and dietary Hg exposure screening benchmarks derived specifically for this assessment. HgPREY exceeded benchmark thresholds related to impaired productivity and behavior in adult loons at 10% and 36% of sites, respectively, and exceeded benchmark thresholds for impaired reproduction and health in fishes at 82% and 73% of sites, respectively. The ecozones of southeastern Canada characterized by extensive forest cover, elevated Hg deposition, and poorly buffered soils had the greatest proportion of RQs > 1.0. Results of this assessment suggest that common loons and piscivorous fishes would likely benefit from reductions in Hg deposition, especially in southeastern Canada.