High‐energy electropulsing triggers recrystallization and phase transformation via excessive Joule heating, potentially causing unwanted damage and compromising the bulk microstructure. Herein, a non‐destructive, low‐energy electric current strategy, termed electroshock treatment (EST), is developed to strengthen grain boundaries (GBs), the preferential site for crack initiation and propagation, while preserving the bulk microstructure. Using α‐Ti as a model system, this strategy achieves a synergistic enhancement of strength and ductility by transforming the defect‐rich GB structure into an ordered atomic arrangement. In situ micropillar compression tests confirm a significant increase in GB strength after EST, while molecular dynamics (MD) simulations reveal that ordered GBs, owing to their lower density of defects, raise the critical stress for dislocation emission and exhibit greater resistance to intergranular fracture. Additionally, a reduction in dislocation density after EST contributes to enhanced ductility. These findings provide a promising GB‐structure‐engineering pathway to reinforce polycrystalline metallic materials.

Hot-deformation pre-bonding is a newly developed method to avoid smelting defects in large stainless steel billets, in which the high-quality interfacial connection needs to be realized as a key guarantee. In this work, a novel electromagnetic shocking treatment (EST) method, as a special way to apply an external physical field, was proposed to introduce the hot-deformation pre-bonded austenitic stainless steel. It is demonstrated that EST can efficiently optimize the hot-deformation pre-bonded interface and restore the tensile properties of pre-bonded stainless steel within several seconds. The interface healing behaviors induced by EST were analyzed via the in situ observation of an optical micrograph, scanning electron micrograph, as well as electron backscattering diffraction. The optimization of the interface connection is mainly attributed to the fact that EST can act on the interface locally, leading to the healing of voids at the interface accompanied by a reduction in stress and the decomposition of oxide. In addition, EST plays another important role in adjusting the texture difference at both ends of the interface, which can further improve the mechanical properties. The results suggest that EST exhibits great potential in promoting the hot-deformation pre-bonding of large billets.