The focus of this study is to investigate processes causing the observed spatial variation of total mercury (THg) in the soil O horizon of watersheds within the Superior National Forest (Minnesota) and to determine if results have implications toward understanding long-term changes in THg concentrations for resident fish. Principal component analysis was used to evaluate the spatial relationships of 42 chemical elements in three soil horizons over 10 watersheds. Results indicate that soil organic carbon is the primary factor controlling the spatial variation of certain metals (Hg, Tl, Pb, Bi, Cd, Sn, Sb, Cu, and As) in the O and A soil horizons. In the B/E horizon, organic carbon appeared to play a minor role in metal spatial variation. These characteristics are consistent with the concentration of soil organic matter and carbon decreasing from the O to the B/E horizons. We also investigated the relationship between percent change in upland soil organic content and fish THg concentrations across all watersheds. Statistical regression analysis indicates that a 50% reduction in age-one and age-two fish THg concentration could result from an average 10% decrease in upland soil organic content. Disturbances that decrease the content of THg and organic matter in the O and A horizons (e.g., fire) may cause a short-term increase in atmospherically deposited mercury but, over the long term, may lead to decreased fish THg concentrations in affected watersheds.