The development of high-performance nonprecious electrocatalysts for overall water splitting has attracted increasing attention but remains a vital challenge. Herein, we report a ZnO-based template method to fabricate Ni nanotube arrays (NTAs) anchored on nickel foil for applications in the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). On the basis of this precursor electrode, the three-dimensional NiSe2 NTAs of unique sandwich-like coaxial structure have been fabricated by electrodeposition of NiSe2 on Ni NTAs, which exhibits high performance toward the HER in both acidic and alkaline media. The method based on Ni NTAs can be readily extended to fabricate Ni2P NTAs by gas–solid phosphorization for the HER, and NiFeOx NTAs by anodic codeposition of Ni and Fe for the OER. Consequently, an alkaline electrolyzer has been constructed using NiFeOx NTAs and NiSe2 NTAs as anode and cathode, respectively, which can realize overall water splitting with a current density of 100 mA cm–2 at an overpotential of 510 mV.