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Few land disturbances impact watersheds at the scale and extent of mountaintop removal mining (MTM). This practice removes forests, soils and bedrock to gain access to underground coal that results in likely permanent and wholesale changes that impact catchment hydrology, geochemistry and ecosystem health. MTM is the dominant driver of land cover changes in the central Appalachian Mountains region of the United States, converting forests to mine lands and burying headwater streams. Despite its dominance on the landscape, determining the hydrological impacts of MTM is complicated by underground coal mines that significantly alter groundwater hydrology. To provide insight into how coal mining impacts headwater catchments, we compared the hydrologic responses of an MTM and forested catchment using event rainfall-runoff analysis, modeling and isotopic approaches. Despite similar rainfall characteristics, hydrology in the two catchments differed in significant ways, but both catchments demonstrated threshold-mediated hydrologic behavior that was attributed to transient storage and the release of runoff from underground mines. Results suggest that underground mines are important controls for runoff generation in both obviously disturbed and seemingly undisturbed catchments and interact in uncertain ways with disturbance from MTM. This paper summarizes our results and demonstrates the complexity of catchment hydrology in the MTM region.