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Electrocatalytic O2 conversion and water-splitting hold great promise to enable the chemicals–electricity inter-transition in many renewable-energy initiatives. Enhancing the kinetics of the oxygen reduction reaction (ORR) is challenging. Here, we present that Zn3(VO4)2/Ni(OH)2/rGO (reduced graphene oxide) nanosheet arrays-a Zn3(VO4)2/Ni(OH)2 composite in the form of nanometre-thick nanosheets on an rGO substrate-serve as an efficient and stable electrocatalyst for the ORR in alkaline electrolytes. The thin-sheet structure and smaller free energy of Zn3(VO4)2/Ni(OH)2, as well as the excellent conductivity of the rGO substrate, enable a large electrochemically-active surface area and a high electron transport, contributing to the superior electrocatalytic oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER). Furthermore, Zn3(VO4)2/Ni(OH)2/rGO and Zn3(VO4)2/Ni(OH)2 samples exhibit remarkable long-term water-splitting stability of 48 h. Density functional theory (DFT) calculations reveal the optimized intermediate affinity ability at the Ni(OH)2 side, due to electrons transferring from Ni(OH)2 to Zn3(VO4)2. Additionally, the higher hybridization degree of density of states (DOS) boosts electron transfer in the electrocatalytic process. More broadly, this work provides new inspiration for the construction of a novel noble metal-free electrocatalyst that could show great promise in energy electrocatalysis. [ABSTRACT FROM AUTHOR]