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To improve the complexity and low catalytic performance and reduce the high cost of the traditional electrode preparation process for the sodium borohydride electro-oxidation reaction (BOR), in this work, a self-supported and efficient electrode material grown on nickel foam (CoNi/Co3O4/NF) was successfully designed using a simple hydrothermal synthesis method accompanied by the electrodeposition process. Benefiting from the three-dimensional nanoarray structure of CoNi/Co3O4/NF and the uniform distribution of Co and Ni modulating active sites by electrodeposition, the catalytic activity towards NaBH4 exhibits high efficiency. CoNi/Co3O4 exhibits excellent catalytic performance (up to 2157 mA cm−2 in 2 mol L−1 NaOH and 0.3 mol L−1 NaBH4), a high electrochemically active surface area (62.5 cm−2), and a low activation energy (15.56 kJ mol−1). The CoNi/Co3O4/NF electrode was further investigated on a direct sodium borohydride–hydrogen peroxide fuel cell (DBHPFC), which exhibited a maximum power density of 108.5 mW cm−2 and excellent stability. The excellent performance is mainly due to its unique nanoarray structure and electrodeposition distribution of Co and Ni active sites, which increases the electrochemical surface area and enhances the contact between the electrode and the electrolyte. [ABSTRACT FROM AUTHOR]