capsulating the electrocatalysts. [27,[43][44][45][46] Recently, Zhao and coworkers [47] and Dai and co-workers [48,49] anchored Co, Ni-Fe based water splitting catalysts on multiwall carbon nanotubes (MWCNTs), these approaches not only enhanced the charge transportations but also increased the available catalytic sites. Although the obtained materials exhibit excellent activity toward water oxidation, the improvement are not significant compared to the original catalysts. Very recently, Zhao and co-workers [50] reported a metal free catalyst based on oxidized MWCNTs (O-MWCNTs) which shows comparable activities to the transition metal-based catalysts, due to the generated oxygen containing ketone groups on surface. This work inspired us to revisit the inorganic/nanocarbon hybrid materials in pursuit of more advanced OER electrocatalysts.As desired, a surprisingly high active OER catalyst has been obtained by simply anchoring the crystalline β−Ni(OH) 2 onto the O-MWCNTs. Different from previous studies, this is the first time that a hybrid material with low Ni contents exhibits extremely high activities for catalyzing oxygen evolution. [41,46] This work paves the path for designing new earth abundant material based alternatives to replace the benchmarking precious Ir/Ru OER catalysts.In order to densely embed the Nickel hydroxide on the MWCNT S , a two-step synthetic strategy was employed to synthesize the hybrid materials as shown in Figure 1. First, the as purchased MWCNTs were purified and mildly oxidized by a piranha solution followed by hydrothermal treatment according to the literature method. [50] Afterward, the freshly obtained O-MWCNTs were mixed with the hydrolysed Ni 2+ solution to afford the hybrid materials. NH 4 OH was introduced as the precipitating reactant instead of strong alkali solution to obtain a particularly pure nickel hydroxide. [51] To gain insights into how the Ni contents in the hybrid materials affect the efficiency toward catalytic water oxidation, five samples with various Ni contents were prepared following the same synthetic route (see the Supporting Information).To gain insight into the structure, morphologies, and composition of the synthesized materials, powder X-ray diffraction (PXRD), scanning electron microscopy, transmission electron microscopy (TEM), hard X-ray photoelectron spectroscopy measurements (HAXPES) and, thermogravimetry (TG) techniques were used to characterize these materials. The morphology of the O-MWCNTs was determined by TEM, as shown in Figure S2a in the Supporting Information. After the loading of Ni, PXRD, and HAXPES (Figure 2a and Figure 3) show that the obtained catalysts are composed of pure crystalline β-Ni(OH) 2 and O-MWCNTs, moreover, no metal impurities such as Fe and Co were detected ( Figure S1, SupportingThe rapid growth in energy demand, the continuous consumption of fossil fuels and the arising environmental concerns are stimulating significant research interests in developing alternative energy systems. [1] Production of hydrogen from electro...