To assess the groundwater−river water interaction in a point-bar alluvial aquifer as a crucial step in site assessment for riverbank filtration, hydrochemical and hydrogeologic investigations were performed on a riverine island at the low reach of the Nakdong River, South Korea. The site was evaluated for the application of large-scale bank filtration. Unconsolidated sediments (~40 m thick) of the island comprise fine- to medium-grained sand (upper aquifer), silty sand with clay intercalations, and sandy gravel (lower aquifer) in descending order. The intermediate layer represents an impermeable aquitard and extends below the river bottom. A total of 66 water samples were collected for this study; groundwater (n = 57) was sampled from both preexisting irrigation wells, and three multi-level monitoring wells (each 35 m deep). Groundwater chemistry is highly variable, but it shows a distinct hydrochemical change with depth: shallow groundwater (<25 m deep) from the upper aquifer is characteristically enriched in NO3− and SO42−, due to agricultural contamination from the land surface, while deeper groundwater (>25 m deep) from the lower aquifer is generally free of NO3− and relatively rich in F. The lower aquifer groundwater is also higher in pH, and concentrations of K+, Mg2+, and HCO3−, indicating that the aquifer is likely fed by regional groundwater flow. Such separation of groundwater into two water bodies is the result of the existence of an impermeable layer at intermediate depth. In addition, the hyporheic flow of river water is locally recognized at the upstream part of the upper aquifer as the zone of low TDS (Total Dissolved Solids) values (<200 mg/L). This study shows that the study site does not seem to be promising for large-scale riverbank filtration because 1) the productive, lower aquifer is not directly connected to the bottom of the river channel, and 2) the upper aquifer is severely influenced by agricultural contamination. This study implies that the subsurface hydrogeologic environment should be carefully investigated for site assessment for riverbank filtration, which can be aided by a detailed survey of groundwater chemistry.