The dataset for the manuscript titled, “Elevated-Mn ChemCam Targets Illuminating Mn Redox Cycling and Diagenesis in the Bradbury Rise, Gale Crater, Mars” consists of a single CSV file. This CSV contains 1,539 rows, with one ChemCam observation point per row. The observation points in this file are from the ChemCam rock targets between martian solar days (sols) 1 and 600 of the MSL Curiosity rover mission that have at least one observation point with > 0.2 wt% MnO. Metadata and compositional data are provided for each row. The metadata includes the LIBS spectrum filename; the name of the target to which the observation point belongs; the class into which we grouped the target; the spacecraft clock value (timestamp) for the observation point; the sol on which the observation was taken; and the ChemCam sequence identifier; the observation point number within the sequence; the ChemCam-to-target distance (in meters); the laser power used for the LIBS measurements; the spectrum totals; and a binary column indicating whether the observation point has > 0.2 wt% MnO. The compositional data includes the oxide chemistry (oxide wt.%), RMSEP accuracy, and shot-to-shot standard deviation, for the major oxides SiO2, TiO2, Al2O3, FeOT, MgO, CaO, Na2O, K2O, as well as for MnO; the sum of oxides for each observation point is also provided.