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High levels of methylmercury accumulation in marine biota are a concern throughout the Arctic, where coastal ocean ecosystems received large riverine inputs of mercury (Hg) (40 Mg·y−1) and sediment (20 Tg·y−1) during the last decade, primarily from major Russian rivers. Hg concentrations in fish harvested from these rivers have declined since the late 20th century, but no temporal data on riverine Hg, which is often strongly associated with suspended sediments, were previously available. Here, we investigate temporal trends in Russian river particulate Hg (PHg) and total suspended solids (TSS) to better understand recent changes in the Arctic Hg cycle and its potential future trajectories. We used 1,300 measurements of Hg in TSS together with discharge observations made by Russian hydrochemistry and hydrology monitoring programs to examine changes in PHg and TSS concentrations and fluxes in eight major Russian rivers between ca. 1975 and 2010. Due to decreases in both PHg concentrations (micrograms per gram) and TSS loads, annual PHg export declined from 47 to 7 Mg·y−1 overall and up to 92% for individual rivers. Modeling of atmospheric Hg deposition together with published inventories on reservoir establishment and industrial Hg release point to decreased pollution and sedimentation within reservoirs as predominant drivers of declining PHg export. We estimate that Russian rivers were the primary source of Hg to the Arctic Ocean in the mid to late 20th century.