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Although great efforts have been devoted to the size\u2010, shape\u2010, and architecture\u2010controlled synthesis of noble\u2010metal nanomaterials, their crystal\u2010phase\u2010controlled synthesis is still in its infancy. Here, for the first time, this study reports high\u2010yield synthesis of Au nanorods (NRs) with alternating 4H\/face\u2010centered cubic (fcc) crystal\u2010phase heterostructures via a one\u2010pot wet\u2010chemical method. The coexistence of 4H and fcc phases is relatively stable, and the 4H\/fcc Au NRs can serve as templates for crystal\u2010phase\u2010controlled epitaxial growth of other metals. As an example, bimetallic 4H\/fcc Au@Pd core\u2013shell NRs are synthesized via the epitaxial growth of Pd on 4H\/fcc Au NRs. Significantly, the 4H\/fcc Au@Pd NRs show superior mass activity toward the ethanol oxidation reaction, i.e., 6.2 and 4.9 times those of commercial Pd black and Pt\/C catalysts, respectively. 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