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Grain boundary diffusion (GBD) of multiple rare earths has proven effective in enhancing the performance of permanent magnets, whereas the diffusion behaviors are still unclear due to their intricate interactions. In this work, the synergistic effects of three rare earths (Tb, Ce, and La) on the grain boundaries diffusion process are investigated, achieving a high‐performance diffused Nd–Fe–B magnet with the high coercivity of 1822 kA m−1 and thermal stability of −0.447% K−1. This promotion originates from the improved diffusion depth of Tb at specific regions, induced by the coordination effects of Ce and La, as evidenced via electron probe microanalysis and the first‐principles calculations. It thus results in the uniform formation of Tb‐diffused magnetic harden grains, associated with the strongly pinned domain walls, which is further observed directly by in situ Lorentz transmission electron microscopy and reconstructed by micromagnetic simulations. The study provides insight into the role of element GBD mechanism and has promising potential to explore other element systems as diffusion sources for permanent magnets.

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