Retrogressive thaw slumps (RTSs) are thermokarst features created by the rapid thaw of ice-rich permafrost, and can mobilize vast quantities of sediments and solutes downstream. However, the effect of slumping on downstream concentrations and yields of total mercury (THg) and methylmercury (MeHg) is unknown. Fluvial concentrations of THg and MeHg downstream of RTSs on the Peel Plateau (Northwest Territories, Canada) were up to 2 orders of magnitude higher than upstream, reaching concentrations of 1,270 ng L-1 and 7 ng L-1, respectively, the highest ever measured in uncontaminated sites in Canada. MeHg concentrations were particularly elevated at sites downstream of RTSs where debris tongues dammed streams to form reservoirs where microbial Hg methylation was likely enhanced. However, > 95% of the Hg downstream was typically particle-bound and potentially not readily bioavailable. Mean open-water season yields of THg (610 mg km-2 d-1) and MeHg (2.61 mg km-2 d-1) downstream of RTSs were up to an order of magnitude higher than those for the nearby large Yukon, Mackenzie and Peel rivers. We estimate that ∼5% of the Hg stored for centuries or millennia in northern permafrost soils (88 Gg) is susceptible to release into modern-day Hg biogeochemical cycling from further climate changes and thermokarst formation.