The Great Smoky Mountains in the southeastern U.S. receive high total atmospheric deposition of sulphur and nitrogen (N) and contain large areas of shallow, poorly buffered soils. Results from extensive surveys conducted in October 1993 and March 1994 showed that stream pH values were near or below 5.5 and Acid Neutralizing Capacity (ANC) was below 50 peq'L q at high elevations. Mechanisms of acidification varies among stream systems in the study. We classified each study caflclunent into one of five water quality districts based upon within-basin elevational gradients of streamwater quality. Geologic factors, cf. the presence of calcareous or pyritic bedrock types exhibited a major influence on water quality and within-basin elevational gradients. Atmospheric deposition is an imporlant factor affecting water quality at high elevations in all districts. Nitrate was the dominant strong acid anion in streamwater in many catchments, particularly at high elevation and especially in basins draining old growth forests. Most high elevation catchments appear to be N satmated. Continued high atmospheric loadings of N will likely spread N saturation of catchments downslope into areas where second growth forests are now malming~ Stream sulphate concentrations were lower than expected at higher elevations and may be related to the N saturation slams of these systems.