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• Hierarchically multi-branched PdRuCu NAs were prepared by a one-step aqueous method. • NP-40 and NaBr as co-directing agents had synergistic effects in the formation of the specific architectures. • The hierarchically multi-branched nanostructures had the large ECSA. • The PdRuCu NAs showed the superior catalytic activity and stability towards EOR and EGOR. Shaped-controlled synthesis of high-efficiency electrocatalysts towards ethanol oxidation reaction (EOR) and ethylene glycol oxidation reaction (EGOR) is important for development of alcohol alkaline fuel cells. Herein, one-step aqueous method was developed for constructing hierarchically multi-branched PdRuCu nanoassemblies (NAs) under the guidance of octylphenoxypolyethoxyethanol (NP-40) and NaBr. The as-obtained PdRuCu NAs exhibited dramatically enhanced electrocatalytic activity and improved stability for EOR and EGOR in alkaline solution. The mass/specific activity of the as-prepared catalysts for EOR (1.16 A mg−1 Pd /3.78 mA cm−2) and EGOR (1.29 A mg−1 Pd /4.19 mA cm−2) were steeply higher than those of commercial Pd black (0.17 A mg−1 Pd /1.81 mA cm−2; 0.21 A mg−1 Pd /2.27 mA cm−2), respectively. This work would provide some valuable insights for synthesis of advanced polymetallic electrocatalysts in fuel cells. [ABSTRACT FROM AUTHOR]