Evaporite salts are abundant around the McMurdo region, Antarctica (∼78°S) due to very low precipitation, low relative humidity, and limited overland flow. Hygroscopic salts in the McMurdo Dry Valleys (MDVs) are preferentially formed in locations where liquid water is present in the austral summer, including along ephemeral streams, ice-covered lake boundaries, or shallow groundwater tracks. In this study, we collected salts from the Miers, Garwood, and Taylor Valleys on the Antarctic continent, as well as around McMurdo Station on Ross Island in close proximity to water sources with the goal of understanding salt geochemistry in relationship to the hydrology of the area. Halite is ubiquitous; sodium is the major cation (ranging from 70%–90% of cations by meq kg-1 sediment) and chloride is the major anion (>50%) in nearly all samples. However, a wide variety of salt phases and morphologies are tentatively identified through scanning electron microscopy (SEM) and X-ray diffraction (XRD) work. We present new data that identifies trona (Na3(CO3)(HCO3)·2H2O), tentative gaylussite (Na2Ca(CO3)2·5H2O), and tentative glauberite (Na2Ca(SO4)2) in the MDV, of which the later one has not been documented previously. Our work allows for the evaluation of processes that influence brine evolution on a local scale, consequently informing assumptions underlying large-scale processes (such as paleoclimate) in the MDV. Hydrological modeling conducted in FREZCHEM and PHREEQC suggests that a model based on aerosol deposition alone in low elevations on the valley floor inadequately characterizes salt distributions found on the surfaces of the soil because it does not account for other hydrologic inputs/outputs. Implications for the salt distributions include their use as tracers for paleolake levels, geochemical tracers of ephemeral water tracks or “wet patches” in the soil, indicators of chemical weathering products, and potential delineators of ecological communities.