The grain boundary diffusion process employing a mixed diffusion source, comprising heavy rare-earth elements and low-melting metals, significantly enhances the coercivity (Hcj) of sintered Nd-Fe-B magnets. In the present study, Tb and Ga were deposited onto the surface of Nd-Fe-B magnets to serve as a diffusion source for improving hard magnetic properties. The effects of varying deposition sequences of Tb and Ga on the magnetic properties and microstructure of the magnets were analyzed. The findings demonstrate that TbF3 grain boundary diffusion facilitated by Ga effectively increases the efficiency of Tb substitution, leading to enhanced coercivity. When Tb and Ga are deposited simultaneously, coercivity shows a notable improvement of 53.15% compared to the untreated magnet, with no reduction in remanence. Additionally, thermal stability is enhanced, resulting in superior overall magnetic properties. Microstructural analysis reveals that Ga promotes the diffusion of Tb into the magnet. In the magnet where Tb and Ga are co-deposited, the formation of a thinner and more uniform (Nd,Tb)2Fe14B shell-core structure, along with the greater infiltration depth of Tb, leads to a broader distribution of core-shell structures within the magnet. This effectively increases the anisotropy fields (HA) of the main phase grains, preventing the nucleation of antiferromagnetic domains at the edges of main-phase grains, thereby enhancing coercivity. Furthermore, the corrosion resistance of the magnet subjected to mixed diffusion is improved. This study provides a foundation for producing highly efficient magnets with a lower content of heavy rare-earth elements. The simplicity and flexibility of the process make it highly suitable for industrial applications.