Despite recent decreases in atmospheric acid deposition, many watersheds of Great Smoky Mountains National Park (GRSM) have lacked expected corresponding increases in stream water pH. Dissolved organic carbon (DOC) concentrations in stream waters have drawn attention as the possible cause. DOC contributions to stream waters are a major portion of watershed carbon cycling with known influences on broad water quality parameters, such as acidity, nutrients, and dissolved metals (Evans, 2005; Lawrence, 2013). Lawrence & Roy (2020) noted that increased ionic strength within the soil matrix during acidification compressed the diffuse layer which reduced organic carbon solubility and enhanced aggregation of organic matter which has been reversed by the recent reductions in acid deposition. However, whether this biogeochemical process dominates stream acidity is dependent on many potential watershed factors, such as vegetative cover conditions, elevation, slope and soil type, depth and chemistry. Because of the substantial reduction in acid deposition in GRSM, there is a need to investigate this potential concept and better understand the current streamwater quality conditions. Water sampling and data collection are being conducted in a similar manner of past research by focusing on large-scale influencers including topography, geology, pedology and climate (Neff, 2013). Additionally, comparisons of DOC with other chemical constituents, namely inorganic acids and base cations, will provide a better understanding of the biogeochemical relationships. Ultimately, development of predictive models generated from this research would provide a useful tool for the comprehensive approach to natural resource maintenance being undertaken by GRSM management departments.