Tailings ponds created during industrial bitumen extraction from the Athabasca Oil Sands Region (AOSR), Alberta, Canada, have been shown to contain numerous contaminants, such as polycyclic aromatic compounds and naphthenic acids, and to slowly leak into adjacent ground and surface waters. Despite elevated concentrations of total mercury (THg) in nearby Athabasca River waters downstream of the AOSR developments, to date there are no published studies of THg or methylmercury (MeHg; a potent neurotoxin) in the AOSR tailings ponds. Here we present concentrations of THg and MeHg, as well as various water chemistry parameters, within four AOSR tailings ponds. Concentrations of SO₄²⁻, NH₃, Na, and Cl were elevated in tailings ponds relative to nearby freshwaters. Surface water concentrations of THg (filtered: 0.15–0.57 ng/L) and MeHg (unfiltered: <0.02–0.53 ng/L; filtered: <0.02–0.32 ng/L), though, were generally low in the tailings ponds, with the highest concentrations observed in the oldest pond. In the mature fine tailings that settle out in the ponds, concentrations of THg (37.0–197 ng/g) and MeHg (0.10–0.52 ng/g) were also low, with the highest concentrations again in the oldest pond. We calculated that if all the dissolved THg and MeHg potentially leaking annually from the tailings ponds entered the nearby Athabasca River, river THg and MeHg concentrations would increase by only 0.01% and 0.03%, respectively. Overall, these ponds are likely not significant sources of THg or MeHg to nearby ground and surface waters, although due to the potential for Hg methylation to occur in the ponds themselves, other tailings ponds in the AOSR should be monitored to ensure that concentrations of MeHg in them are also low.