Besides radiation resistance, thermal recovery of radiation damage provides another critical criterion to evaluate the host phase for immobilizing high-level waste (HLW) produced by nuclear plants. Despite the increasing investigations, a comprehensive atomic-scale understanding remains elusive on thermal annealing of radiation damage in ceramics. Here, using in situ heating high-resolution transmission electron microscopy, we investigate the thermal annealing of radiation damage in natural metamict titanite (CaTiSiO5) caused by a high alpha decay dose from the incorporated U and Th during the geologic time. The recovery of the fully amorphous titanite precursor starts at 456 ℃ from the appearances of monoclinic nanoparticles 2–5 nanometers wide, and more nanoparticles form as the temperature gradually increases. At 1000 ℃, the amorphous phase recovers through epitaxial growth with titanite nanoparticles as templates. This study provides information for a unit-cell-scale understanding of the thermal stability of radiation damage in titanite-based ceramics, having significance for immobilizing HLW.