Lead isotope compositions of soils and near-surface tills from an area of coastal Maine known to have groundwater with anomalously high arsenic contents were measured in order to determine the source of the lead and, by inference, possible sources of arsenic. Five soil and till sites were selected for detailed chemical and isotopic analysis. To construct profiles of the soil and till horizons, five samples were collected at 10-cm intervals from the surface to the base of each horizon. Total lead and arsenic concentrations and lead isotopic compositions were measured for 48 leaches and bulk residues. The soils and tills are underlain by sulfidic schists of the Penobscot Formation. Several generations of minerals containing arsenic and lead exist in the regional bedrock, including rock-forming silicates (feldspar and micas), sulfide minerals formed during diagenesis (for example, arsenic-rich pyrite), and sulfide and oxide minerals that formed as a result of Silurian metamorphic and igneous events (for example, arsenopyrite, galena, iron-oxides, and arsenic-sulfides). A young group of secondary minerals (for example, iron-hydroxides, arsenic-hydroxides, lead-sulfate, and arsenic-jarosite) formed from recent weathering and pedogenic processes.