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Isle Royale, in Lake Superior, contains evidence of indigenous copper mining; however, the timing and geographical extent of mining activity is poorly known. We analyzed metal, carbon, nitrogen, and organic matter concentrations to document past mining pollution in sediment cores recovered from McCargoe Cove; a long, narrow inlet of Lake Superior on Isle Royale that receives drainage from a watershed that contains numerous ancient copper mines. At McCargoe Cove, concentrations of lead, copper, and potassium increase in the sediments after ad 1860 and between 6500 and 5400 years before ad 1950 (yr BP). Metal pollution increases at McCargoe Cove exceed natural (or background) levels and coincide with radiocarbon dates associated with copper artifacts and existing lead pollution reconstructions from lakes on the Keweenaw Peninsula. Interestingly, a coherent cessation of lead emissions at multiple study sites after ~5400 yr BP coincides with the onset of dry conditions found in regional paleoclimate proxy records. After ~5000 yr BP, lead concentrations on both Isle Royale and the Keweenaw Peninsula remain at background levels until the onset of modern lead pollution ~ad 1860. [ABSTRACT FROM PUBLISHER]