Pegmatites are a major host of global lithium, cesium, and rubidium resources. However, the existing grade and tonnage dataset for lithium pegmatites that was published in 1992 does not represent the current industry parameters used to delineate resources. There are no existing grade and tonnage datasets for cesium and rubidium. We present grade and tonnage data for lithium, cesium, and rubidium mineral resources related to pegmatite deposits. This compilation does not include pegmatite deposits with primary tin or tantalum resources, but we do report tin and tantalum concentrations for lithium-dominated deposits where available. Over 100 potential pegmatite resources were evaluated; however, final selection was limited to resources that were sufficiently delineated in 3-dimensions to define the in-situ resource. The dataset is not an exhaustive list of known pegmatite prospects and deposits but instead aims to capture the current global distribution of in-situ grade and tonnage. The dataset includes two lithium pegmatite deposits in the United States, both in North Carolina. Other known domestic lithium pegmatite resources exist but were excluded because they lack industry-compliant resource estimates. These data can be used for lithium, cesium, and/or rubidium mineral resource assessments or supply chain studies. The global lithium pegmatite dataset is sufficiently large for quantitative mineral resource assessments, depending on underlying assumptions of the assessment. We include a separate comma-delimited text file of lithium pegmatite deposits that is pre-formatted as input for probabilistic simulations of undiscovered deposits in the R-based software package MapMark4. Note that MapMark4 users should evaluate the lithium deposit dataset closely to verify the dataset agrees with the deposit type for which they have estimated undiscovered deposits. While an effort was made to isolate lithium-dominated resources for ease of MapMark4 input, note that some deposits have multiple commodities whereas others are solely lithium resources. These factors should be considered, and references for relevant records evaluated, prior to fitting grade and tonnage models. The three-digit ID field can be used as a primary key to link records from the main compilation to the MapMark4-ready dataset.