Tristructural isotropic (TRISO)-coated fuel particles are designed for use in high-temperature gas-cooled nuclear reactors, featuring a structural SiC layer that may be exposed to oxygen-rich environments over 1000 °C. Surrogate TRISO particles were tested in 0.2–20 kPa O2 atmospheres to observe the differences in oxidation behavior. Oxide growth mechanisms remained consistent from 1200–1600 °C for each PO2, with activation energies of 228 ± 7 kJ/mol for 20 kPa O2 and 188 ± 8 kJ/mol for 0.2 kPa O2. At 1600 °C, kinetic analysis revealed a change in oxide growth mechanisms between 0.2 and 6 kPa O2. In 0.2 kPa O2, oxidation produced raised oxide nodules on pockets with nanocrystalline SiC. Oxidation mechanisms were determined using Atom probe tomography. Active SiC oxidation occurred in C-rich grain boundaries with low PO2, leading to SiO2 buildup in porous nodules. This phenomenon was not observed at any temperature in 20 kPa O2 environments.