Glauconite-bearing deposits are found worldwide, but As levels have been determined for relatively few. The As content of glauconites in sediments of the Inner Coastal Plain of New Jersey can exceed 100 mg/kg, and total As concentrations (up to 5.95 μg/L) found historically and recently in streamwaters exceed the State standard. In a major watershed of the Inner Coastal Plain, chemical “fingerprints” were developed for streambed sediments and groundwater to identify contributions of As to the watershed from geologic and anthropogenic sources. The fingerprint for streambed sediments, which included Be, Cr, Fe and V, indicated that As was predominantly of geologic origin. High concentrations of dissolved organic C, nutrients (and Cl⁻) in shallow groundwater indicated anthropogenic inputs that provided an environment where microbial activity released As from minerals to groundwater discharging to the stream. Particulates in streamwater during high flow constituted most of the As load; the chemical patterns for these particulates resembled the geologic fingerprint of the streambed sediments. The As/Cr ratio of these suspended particles likely indicates they derived not only from runoff, but from groundwater inputs, because As contributed by groundwater is sequestered on streambed sediments. Agricultural inputs of As were not clearly identified, although chemical characteristics of some sediments indicated vehicle-related inputs of metals. Sediment sampling during dry and wet years showed that, under differing hydrologic conditions, local anthropogenic fingerprints could be obscured but the geologic fingerprint, indicating glauconitic sediments as an As source, was robust.