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Surface coal mining is the dominant form of land cover change in Central Appalachia, yet the extent to which surface coal mine runoff is polluting regional rivers is currently unknown. We mapped surface mining from 1976 to 2005 for a 19,581 km2 area of southern West Virginia and linked these maps with water quality and biological data for 223 streams. The extent of surface mining within catchments is highly correlated with the ionic strength and sulfate concentrations of receiving streams. Generalized additive models were used to estimate the amount of watershed mining, stream ionic strength, or sulfate concentrations beyond which biological impairment (based on state biocriteria) is likely. We find this threshold is reached once surface coal mines occupy >5.4% of their contributing watershed area, ionic strength exceeds 308 μS cm–1, or sulfate concentrations exceed 50 mg L–1. Significant losses of many intolerant macroinvertebrate taxa occur when as little as 2.2% of contributing catchments are mined. As of 2005, 5% of the land area of southern WV was converted to surface mines, 6% of regional streams were buried in valley fills, and 22% of the regional stream network length drained watersheds with >5.4% of their surface area converted to mines.