Supplementary dataset and figures accompanying a paper entitled “Improving the Accessibility and Efficiency of Proton Irradiations for 4He/3He Thermochronology” submitted to Geochemistry, Geophysics, Geosystems. The dataset contains 4He/3He step-heating measurements on internal shards of Durango apatite that underwent proton irradiation at three different facilities: the Francis H. Burr Proton Therapy Center (FHB), the Helmholtz Zentrum Berlin (HZB), and the Paul Scherrer Insitute (PSI). Furthermore, the dataset contains bulk 4He and 3He concentrations for each shard analyzed. The supplementary figures include 4He/3He release spectrum plots for each Durango shard analyzed, 3He concentration maps from the HZB irradiation, and detailed results of PHITS simulations used to assess the HZB irradiations.