Concentration variations of sodium (N+). chloride (Cl-). and dissolved silica (H4SiO4) in rainfall, throughfall, soil water, groundwater and streamwater were evaluated at the Panola Mountain Research Watershed near Atlanta, Georgia, to determine how variations in concentrations of these solutes provide greater understanding of water quality evolution at the hillslope and catchment scales Stormwater moves rapidly to depth along preferred pathways in a deciduous forest hillslope, but the composition of the mobile unsaturated zone water in the hillslope is not reflected in compositional variations of streamwater during rainstorms. The Na+, Cl-, and H4SiO4 concentrations behave similarly in streamwater, decreasing with increasing discharge and increasing with water residence time. Consequently, the lowest flows are associated with the highest concentrations and the oldest water. Streamwater composition is most similar to groundwater and stormflow variations reflect a dilution of groundwater. Subtle differences in the relations among solute concentrations and discharge reflect different sources, especially for Cl-. For example, the residence time of groundwater, as inferred from landscape position, generally is positively related to Na+ and H4SiO4 concentrations, but not to Cl- concentrations. The Na+ and H4SiO4 are derived from mineral weathering and are continuously supplied along hydrological pathways. In contrast, Cl- is derived from atmospheric deposition and is affected only by evapotranspiration (ET) and transport. ET increases Cl- concentrations in matrix soil waters, which are subsequently transported to the saturated zone where Cl- is effectively isolated from further evaporative concentration.