Trace element biogeochemistry from soils to rivers is important for toxicity to aquatic ecosystems. The objective of this study was to determine whether trace element exports in contrasting watersheds are controlled by their abundance in soil, current land uses in the watershed, or geologic processes. Upland soils and river water samples were collected throughout the Deerfield watershed in southern Vermont and western Massachusetts and in the Quinebaug and Shetucket watersheds of eastern Connecticut. Soil concentrations were only an important predictor for dissolved Fe export, but no other trace element. Soil pH was not correlated with normalized dissolved exports of trace elements, but DOC was correlated with normalized dissolved Pb and Ni exports. The limited spatial and depth of soil sampling may have contributed to the poor correlation. Surprisingly, linear regressions and principal component analysis showed that human development was associated with higher soil trace metal concentrations but not significantly correlated with dissolved trace elements export. Instead, forest abundance was a strong predictor for lower Cu, Pb, and Zn soil concentrations and lower As, Fe, Ni and Pb dissolved exports across the watersheds. Dissolved exports of Al, K, and Si suggest that enhanced mineral dissolution in the montane watersheds was likely an important factor for matching or exceeding normalized pollutant trace element exports in more urbanized watersheds. Further studies are needed to evaluate subsurface/hyporheic controls as well as soil–surface water interface to quantify exchange and transport.