Lithium demand is projected to increase more than 48 times by 2040 due to electric vehicle production and other energy storage needs. Most lithium production is outside of the USA, thereby increasing supply chain vulnerability. The combined end use importance and heightened supply risk of lithium make this lightest metallic element a critical commodity to the USA. To mitigate this supply risk, the US Geological Survey is actively assessing lithium deposits in the USA. Herein, we detail an assessment for lithium-mineralized pegmatites in the US northern Appalachian Mountains. Permissive tracts were generated by cross-referencing tectonic and geologic maps and mineral occurrence data with mappable criteria derived from generalized and region-specific lithium pegmatite ore deposit models; tracts were then ranked as having high, medium, or low permissibility. Available geophysical and geochemical data were found to be of minimal utility for this deposit type at the scale of the assessment. The number of undiscovered deposits were estimated and integrated into probabilistic simulations, which included an expanded and updated global grade and tonnage model of pegmatite-hosted lithium ore. The estimated total amount of undiscovered resources for the northern Appalachian Orogen has a median value of 1,410,000 metric tons of Li₂O when considering moderate correlation across sub-regions. At a confidence level of 90%, a resource of at least 90,000 metric tons of Li₂O remains undiscovered, and at a 10% confidence level, a resource of as much as 7,380,000 metric tons Li₂O remains undiscovered. After applying an up-to-date economic filter to convert median contained lithium to recoverable material, a correlated total of 900,000 metric tons of Li₂O may be economically extractable, equating to enough Li₂O to provide the current annual US lithium supply deficit (presently obtained through net imports) for 127 years at 2025 rates of apparent consumption. This period of provision will inevitably shorten with projected increasing consumption rates, emphasizing that further research could be completed to better delineate regions of high lithium resource potential and support exploration and domestic production.