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High-efficiency and economical electrocatalysts for electrochemical water splitting are the core component of the renewable energy conversion. Herein, a simple and economical strategy is described to synthesize a series of metal oxide decorated nitrogen-doped carbon nanotubes materials (N-CNT@Cu–Fe Oxide Alloy NPs) by utilizing carbon nanotubes as the substrate carrier material. Additionally, the polypyrrole (PPy) was served as both the nitrogen resource and the localizing agent to load the Cu–Fe oxide alloy. Moreover, the theoretical and test results indicated that the superior HER and ORR performance is mainly related to the synergistic effect between the nitrogen-doped CNT and metallic oxide alloy. In the series of catalysts we prepared, N-CNT@Cu 1 –Fe 1 Oxide Alloy NPs exhibits more significant catalytic activity and better durability than other catalysts that we synthesized. Meanwhile, the catalyst shows the low Tafel slope of 68.28 mV dec−1 for HER and reaches 10 mA cm−2 at the overpotential of 375 mV. The K–L plot shows that the electron transfer number of N–CNF@Cu 1 –Fe 1 Alloy NPs is 3.43. [Display omitted] • Utilizing a new carbon nanotube as the substrate carrier material. • N-doping and oxide alloy formation can be simultaneously realized. • Polypyrrole as nitrogen source and localizing agent simultaneously. • Electron transfer between FePc and Cu2+ for the formation of metallic precursors. • High electrocatalytic performance for both HER and ORR. [ABSTRACT FROM AUTHOR]