The development of cost-effective Ce-magnets with high Ce content is urgent to realize the vision of cost reduction and performance enhancement. Dual-main-phase Ce-magnets with different Ce content (Ce accounted for the total amount of rare earths is 40%, 50% and 60%) are prepared. The Pr80Al20 (at%) alloy is selected as diffusion source for the three magnets using the grain boundary diffusion technique under the same conditions. The correlation of magnetic properties and microstructures before and after diffusion with different Ce contents are systematically analyzed. According to the EPMA results, the presence of Ce in the magnets facilitates the diffusion of Pr elements along the grain boundaries, which significantly increases the diffusion depth of Pr inside the magnets. As a consequence, the percentage increment of coercivity increase with the Ce content due to the increased diffusion depth. This study provides new insight into the preparation of dual-main-phase Ce-magnets with high Ce content of 40–60%.