Major-element and trace-element concentrations in 76 core samples and seven surface samples of rocks from the Coles Hill uranium deposit and vicinity, Pittsylvania County, south-central Virginia are presented as tabular digital data. The Coles Hill deposit is the largest unmined uranium deposit in the United States. The data were collected to 1) characterize the chemistry of variably uranium-mineralized rock units within the deposit and 2) to compare with the chemistry of un-mineralized surface exposures of the same rock units. Cores were sampled in 2017 by U.S. Geological Survey (USGS) personnel from archived historical collections of the Virginia Museum of Natural History. Core samples were selected based on measurable differences in radioactivity and/or visual differences in alteration, fracturing, and brecciation. Rock units present within the deposit are Leatherwood Granite (granite-gneiss of upper Ordovician age) and Rich Acres Formation (amphibolite of Silurian age).