Ce 2 Fe 14 B compound has a great potential to serve as a novel permanent magnet alternative thanks to the abundant and inexpensive rare-earth element (cerium), while its low magnetocrystalline anisotropy and energy product severely restrict its applications. In this work, a novel strategy combining melt-spinning and electron-beam exposure (EBE) aiming for fabricating high-performance Ce-Fe-B magnetic materials is reported to solve the above-mentioned problem. Remarkably, this strategy facilitates developing a suitable grain boundary configuration without using any additional heavy rare-earth element. Under the optimal EBE condition, the maximum energy product ((BH) max ) of pure Ce-Fe-B alloy is 6.5 MGOe, about four times higher than that obtained after conventional rapid thermal processing method for the same precursor. The enhanced intergranular magnetostatic coupling effect in the EBE sample is validated by mapping the first-order-reversal-curve (FORC) diagrams. The in-situ observation of magnetic domain wall motion for Ce-Fe-B alloy using Lorentz transmission electron microscopy reveals that the boundary layers are very effective in pinning the motion of domain walls, leading to the increased coercivity under EBE, and this pinning effect is further verified by micromagnetic simulations. Our results suggest that CeFeB materials using EBE could be a promising candidate after further processing, which could fill the performance "gap" between hexaferrite and Nd-Fe-B-based magnets.