The Adirondack region of New York has been identified as a hot spot where high methylmercury concentrations are found in surface waters and biota, yet mercury (Hg) concentrations vary widely in this region. We collected stream and groundwater samples for Hg and organic carbon analyses across the upper Hudson River, a 493 km2 basin in the central Adirondacks to evaluate and model the sources of variation in filtered total Hg (FTHg) concentrations. Variability in FTHg concentrations during the growing seasons (May-Oct) of 2007-2009 in Fishing Brook, a 66-km2 sub-basin, was better explained by specific ultra-violet absorbance at 254 nm (SUVA254), a measure of organic carbon aromaticity, than by dissolved organic carbon (DOC) concentrations, a commonly used Hg indicator. SUVA254 was a stronger predictor of FTHg concentrations during the growing season than during the dormant season. Multiple linear regression models that included SUVA254 values and DOC concentrations could explain 75 % of the variation in FTHg concentrations on an annual basis and 84 % during the growing season. A multiple linear regression landscape modeling approach applied to 27 synoptic sites across the upper Hudson basin found that higher SUVA254 values are associated with gentler slopes, and greater riparian area, and lower SUVA254 values are associated with an increasing influence of open water. We hypothesize that the strong Hg?SUVA254 relation in this basin reflects distinct patterns of FTHg and SUVA254 that are characteristic of source areas that control the mobilization of Hg to surface waters, and that the seasonal influence of these source areas varies in this heterogeneous basin landscape.