This study characterizes the mass transport of ions in two streams in the Great Smoky Mountains National Park, comparing transport between stormflow and baseflow periods. By comparing ion mass transport between these two hydrological conditions, the importance of soil and the governing biogeochemical processes will be underscored. Two water quality monitoring study sites were located on the Middle Prong of the Little Pigeon River and Ramsey Prong within the same basin. These remote sites were equipped with YSI 6920 multi-parameter sonde to record continuous 15-min data of pH, depth, conductivity, turbidity, and temperature. Additionally, ISCO 6712 composite samplers were used to collect stream samples during storm events. Baseflow was collected by grab samples prior to storm events, and stormflow collected by ISCO samplers. Throughfall samples were collected after storm events. All samples were analyzed for pH, ANC, and conductivity using an autotitrator. Inductively coupled plasma spectrometry and ion chromatography were used to determine major cations, trace metals, and anions (Ca2+, Na+, K+, Mg2+, Aln+, Cu, Fe, Mn, Si, Zn, SO42-, NO3-, Cl-, NH4+). Stage-discharge relationships were developed at each site utilizing a combination of field measurements and modeling. Velocity and area field measurements were taken to calculate discharges for mid- to low-flow stages while mid- to upper-flow stages were modeled using RIVER2D and verified with field measurements. Stage-discharge curves and sample ion concentrations were used to compute ion mass transport for a two year period in 2006 through 2008. Differences in mass transport of ions between baseflow and stormflow periods found that greater mass transport of ions, except protons, occurred during baseflow periods. These results indicate that on an annual basis ions are stored from input throughfall sources and released gradually through groundwater flow over time more than rapid interflow transport during storm events. This information illustrates the importance of soils and groundwater storage in the regulation of ion transport and streamwater quality in the Great Smoky Mountains National Park.