Pt-based nanomaterials have been proven to be effective catalysts for direct alcohol fuel cells (DAFCs). Specifically, the ternary nanoalloys (NAs) composed of Pt with other noble metals and transition metals can not only reduce the component of Pt but also enhance the electrocatalytic property and durability for alcohol oxidation. Herein, ternary PdPtCu NAs were synthesized through the solvothermal method using ethylene glycol as the solvent and reducing agent. The morphology and composition of PdPtCu NAs can be effectively controlled via selecting suitable surfactants and adjusting the proportion of precursors. The threedimensional (3D) PdPtCu NAs with spiny rambutan-like morphology were obtained using the triblock copolymer Pluronic F-127 (PF-127) as the surfactant and adding three precursors with an equal molar ratio. The unique structure of PdPtCu NAs and the synergistic effect between the components significantly improved the electrocatalytic activity toward ethanol oxidation. Compared with different atomic ratio binary or ternary nanomaterials, 3D PdPtCu NAs manifested the best electrocatalytic performance.