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Developing electrocatalysts with ultrathin nanostructures and high mesoporosity is a relevant high‐priority research direction toward enhancing the performance of noble metals. Herein, mesoporous, highly excavated octahedral PtCu3 nanostructures are prepared by a facile one‐pot synthesis. The mesoporous, highly excavated octahedral PtCu3 nanostructures are built with mutually perpendicular interlaced...