The design of high-efficiency non-noble bifunctional electrocatalysts for oxygen evolution reaction and hydrogen evolution reaction is paramount for water splitting technologies and associated renewable energy systems. Spinel-structured oxides with rich redox properties can serve as alternative low-cost electrocatalysts. However, the spinel-structured oxides is a typical electrocatalyst for OER but with poor HER performance. In this work, zirconium regulation in threedimensional (3D) CoFe 2 O 4 (CoFeZr oxides) nanosheets on nickel foam (NF) as a novel strategy inducing bifunctionality toward OER and HER for overall water splitting is reported. The results demonstrate that the incorporation of Zr into CoFe 2 O 4 can tune the nanosheet morphology and electronic structure around Co and Fe sites for optimizing adsorption energies, thus effectively enhancing the intrinsic activity of active sites. The as-synthesized optimal electrocatalyst of 3D CoFeZr oxides nanosheets exhibited high OER activity with small overpotential, low Tafel slope and good stability. Moreover, the CoFeZr oxide nanosheets showed unprecedented HER activity with a small overpotential of 104 mV at 10 mA cm −2 in alkaline media, which is better than ever reported This article is protected by copyright. All rights reserved.3 spinel-structured oxides. When employing the CoFeZr oxides nanosheets as both anode and cathode catalysts for overall water splitting, a current density of 10 mA cm 2 was achieved at the cell voltage of 1.63 V in 1.0 M KOH. The results demonstrate that such favorable OER and HER activity can be attributed to fast electron transportation, improved electrical conductivity and optimal electronic structure.