Voids are a common issue in cold-sprayed coatings, negatively impacting their mechanical properties and bonding strength. In this study, we report an efficient void healing approach for cold-sprayed coatings via pressure-free low-temperature sintering, and unveil the void healing mechanism at the atomic level. Sintering at 500°C (∼0.59 Tm) for 20 hours effectively reduces the porosity in the cold-sprayed CuCrZr coating, leading to a significant enhancement in shear bonding strength with an Al2O3 dispersion-strengthened copper substrate by a factor of 3.5. It is found that an intermediate nanograined layer formed between the coating and the substrate plays a crucial role in the subsequent void healing process during sintering. This nanocrystalline layer, a byproduct of continuous dynamic recrystallization activated by high strain-rate deformation of powders during cold spray, demonstrates thermal instability and high grain growth capability, thereby accelerating the void healing process. In-situ TEM observations unveil the growth of nanograins along with the in-situ generation of Cr2O3 oxides, gradually filling the voids and contributing to the void healing process. Molecular dynamics simulations indicate that grain boundary (GB) migration in nanograins facilitates atom diffusion, enhancing GB-voids interaction. The GB structural transformation during heating provides an efficient diffusion channel for transporting vacancies, thereby accelerating the closure of voids.