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Building heterostructures is the most promising material design strategy to break through the limitations of oxygen evolution reaction (OER) kinetics and promote efficient hydrolysis. This review focuses on nickel\u2010based heterostructured electrocatalysts, whose interface synergy between different components significantly improves catalytic performance. First, the three basic OER mechanisms were discussed, elucidating the relationship between micro interfaces and mechanisms. Then, the latest developments in different nickel\u2010based material systems reveal how interfacial synergistic effects accelerate charge transfer and regulate intermediate adsorption. In addition, we focused on advanced performance optimization strategies, such as the latest advances in optimizing oxygen evolution performance through doping, defect control, and crystal phase engineering. Finally, we identified the challenges faced by this field in industrial applications and pointed out the integration of in situ characterization, theoretical calculations, and artificial intelligence design to achieve controllable preparation of interface active sites. This review provides important theoretical references for the design and development of a new generation of high\u2010performance and scalable OER electrocatalysts, helping to promote the high\u2010quality development of the green hydrogen energy industry.<\/jats:p>","DOI":"10.1002\/cssc.70860","type":"journal-article","created":{"date-parts":[[2026,7,15]],"date-time":"2026-07-15T04:35:02Z","timestamp":1784090102000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Rational Design of Nickel\u2010Based Heterostructured Electrocatalysts for Oxygen Evolution Reaction: Mechanisms, Advances, and Optimization Strategies"],"prefix":"10.1002","volume":"19","author":[{"ORCID":"https:\/\/orcid.org\/0009-0003-6165-9853","authenticated-orcid":false,"given":"Xinyi","family":"Men","sequence":"first","affiliation":[{"name":"Key Laboratory of Advanced Technologies of Materials, (Ministry of Education) Southwest Jiaotong University  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