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Herein, a non\u2010destructive, low\u2010energy 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 \u03b1\u2010Ti as a model system, this strategy achieves a synergistic enhancement of strength and ductility by transforming the defect\u2010rich 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\u2010structure\u2010engineering pathway to reinforce polycrystalline metallic materials.<\/jats:p>","DOI":"10.1002\/advs.77128","type":"journal-article","created":{"date-parts":[[2026,8,19]],"date-time":"2026-08-19T10:26:26Z","timestamp":1787135186000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["Grain Boundary Structure Ordering via Electroshock Treatment Enhances Strength\u2010Ductility Synergy"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-0650-9310","authenticated-orcid":false,"given":"Jiancheng","family":"Chen","sequence":"first","affiliation":[{"name":"State Key Laboratory of Light Superalloys Wuhan University of Technology  Wuhan China"},{"name":"Department of Mechanical Engineering Research Institute for Advanced Manufacturing The Hong Kong Polytechnic University  Kowloon Hong Kong China"},{"name":"School of Materials Science and Engineering 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