Past investigations at historical gold (Au) districts in Nova Scotia, Canada have identified elevated concentrations of arsenic (As) and mercury (Hg) in nearby sediments and waters. These metal(loid)s are derived from erosion of mineralized bedrock, and the disposal of mine tailings into the environment during early operations. The Wine Harbour gold district is located along the eastern shore of Nova Scotia, and produced 1329 kg of Au from 75 581 tonnes of crushed rock from 1862 to 1939.The gold occurs in arsenopyrite-bearing quartz-carbonate veins and was extracted using stamp milling and Hg amalgamation. Historical maps document tailings deposits near former stamp mill sites; however, the extent to which these mine wastes influence environmental quality in the adjacent marine environment is uncertain. In this study, we measured metal(loid) concentrations in tailings, marine sediments, and surface waters to assess the lateral and vertical extent of mining-related impacts on Wine Harbour. Chemical analyses of terrestrial and intertidal tailings reveal high concentrations of both As (86–196 000 mg/kg) and Hg (444–320 000 µg/kg). Analyses of marine sediments show a wide range in both As (4–568 mg/kg) and Hg (<5–7430 µg/kg) concentrations. In general, the highest metal(loid) concentrations in sediments were recorded down-gradient of stamp mill sites. Elevated concentrations were also detected in sediments underlying an active mussel aquaculture operation at the western end of the harbour. Results from this study have been used to help assess potential ecosystem and human health risks associated with historical gold mine wastes in the Wine Harbour area.