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Palladium-based catalyst represents one of the most promising candidates among all non-platinum oxygen reduction reaction (ORR) catalysts. However, it is still challenging to precisely engineering their morphology and composition. Herein, highly branched core-shell PdCu@Pd nanocrystals have been fabricated via a simple one-pot synthesis that co-directed by hydrogen gas and halide ions. Such unique PdCu@Pd nanocrystals exhibit prominent ORR activity, durability and methanol-tolerance in alkaline media owing to their core-shell composition, highly-branched structure and defect-rich surface. This work elucidates a facile strategy to design highly branched core-shell nanomaterials, shedding light on the exploration and optimization of novel non-platinum ORR catalysts.