The first quantitative mineral resource assessment for undiscovered lithium pegmatite deposits in the southern Appalachian region of the United States was conducted. Permissive tracts for lithium pegmatite deposits were delineated by integrating lithological, tectonic, geochemical, geophysical and mineral occurrence data. Lithium pegmatite prospectivity of the tracts was ranked with simplified mappable criteria, including proximity to Paleozoic felsic intrusions and major lithotectonic structures, stream sediment geochemical anomalies, and pegmatite occurrence data. The geospatial data and permissive tracts were used to estimate the number of undiscovered lithium pegmatite deposits. These estimates were integrated into probabilistic simulations along with a new global lithium pegmatite grade and tonnage dataset to quantify potential contained undiscovered lithium resources. An economic filter was applied to convert the probabilistic estimates of contained lithium into recoverable material. The identified lithium pegmatite resources for the Carolina Lithium and Kings Mountain deposits, North Carolina, contain 1589 thousand tons (kt) of Li₂O. The median contained undiscovered resource for the southern Appalachian orogen was estimated to be 2240 kt Li₂O. At 90% confidence, the region contains at least 130 kt Li₂O, and 10,700 kt at 10% confidence. After applying economic filters, the median recoverable contained resource was 1430 kt Li₂O, corresponding to approximately 201 years of current lithium imports for consumption in the United States. North and South Carolina are likely to contain most of these resources. Coarse data resolution and intra-state variations in the geological data contribute to uncertainty of undiscovered lithium pegmatite resources. Continued efforts to harmonize disparate geospatial datasets with updated or new information can improve the accuracy and precision of estimated undiscovered lithium pegmatite resources in the study area and at broader scales.