Trace elements used in animal feed additives can be introduced to aquatic environments through application of manures from animal feeding operations to agricultural land as fertilizer. The use of poultry feed additives containing arsenic (As) is of particular concern in the Shenandoah River watershed (Virginia, USA), an agricultural landscape with a high density of poultry operations. This study investigated the relationship between watershed characteristics of Shenandoah River tributaries and trace element concentrations in streambed sediment and tissue of resident mollusks, including: Asian clams (Corbicula fluminea), which are commonly used biomonitors, and pleurocerid snails (Leptoxis carinata), which are generally understudied. Results failed to support the primary hypothesis of a predictive relationship between watershed densities of poultry operations and As concentrations in sediment and mollusk tissue. However, there were statistical relationships between land use in tributary watersheds and other trace elements in sediment (Cu, Mn, Pb, Zn) and tissue (Cd, Hg, Pb). Principal components analysis of the sediment data suggested a possible geologic source of As at some sites. Tissue concentrations of As were significantly higher in snails than in clams, but clams accumulated higher concentrations of other trace elements (Cd, Cr, Hg, Pb, Se). Snails may be useful biomonitors of environmental As, but appear to be less suitable than clams for studies of landscape sources of other trace elements.