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Highlights Facile electrodeposition for fabricating active Ni nanodots (NiNDs) on Ni foam (NF) is shown.Binder- and heteroatom-free recyclable NiO/NiNDs@NF electrodes are efficiently made.NiO/NiNDs@NF bifunctional catalytic electrodes are used for water splitting. Electronic supplementary material The online version of this article (10.1007/s40820-019-0269-x) contains supplementary material, which is available to authorized users., In past decades, Ni-based catalytic materials and electrodes have been intensively explored as low-cost hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) catalysts for water splitting. With increasing demands for Ni worldwide, simplifying the fabrication process, increasing Ni recycling, and reducing waste are tangible sustainability goals. Here, binder-free, heteroatom-free, and recyclable Ni-based bifunctional catalytic electrodes were fabricated via a one-step quick electrodeposition method. Typically, active Ni nanodot (NiND) clusters are electrodeposited on Ni foam (NF) in Ni(NO3)2 acetonitrile solution. After drying in air, NiO/NiND composites are obtained, leading to a binder-free and heteroatom-free NiO/NiNDs@NF catalytic electrode. The electrode shows high efficiency and long-term stability for catalyzing hydrogen and oxygen evolution reactions at low overpotentials (10ηHER = 119 mV and 50ηOER = 360 mV) and can promote water catalysis at 1.70 V@10 mA cm−2. More importantly, the recovery of raw materials (NF and Ni(NO3)2) is quite easy because of the solubility of NiO/NiNDs composites in acid solution for recycling the electrodes. Additionally, a large-sized (S ~ 70 cm2) NiO/NiNDs@NF catalytic electrode with high durability has also been constructed. This method provides a simple and fast technology to construct high-performance, low-cost, and environmentally friendly Ni-based bifunctional electrocatalytic electrodes for water splitting. Electronic supplementary material The online version of this article (10.1007/s40820-019-0269-x) contains supplementary material, which is available to authorized users.