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Hydrogen energy is clean and serves as one of the most promising candidates for replacing petroleum fuels in the future. Although the rare metals, such as platinum, have high efficiency in the hydrogen evolution reaction (HER), their scarcity and high cost inhibit large scale applications.[1–6] Recently, inorganic catalysts such as nanometer-scaled MoS 2 and WS 2 have drawn great attention due to their low cost, high chemical stability, and excellent photocatalytic [7–24] and electrocatalytic properties in HERs. They are potentially useful if they can be tailored for the development of hydrogen energy devices. In order to enhance the efficiency of inorganic catalysts, many research efforts have been made toward the modification of material properties,[25] the formation of composite catalysts,[26–31] and the fabrication of the electrodes with nano-architecture.[30–33] Recently, MoS 2/reduced graphene oxide catalyst composites have been successfully made for enhancing the electrocatalytic HER efficiency, where the reduced graphene oxide sheets serve the function of hosting MoS 2 as well as enhancing the conductance of the composites.[31, 34] However, most of the reported electrode materials were still based on two-dimensional (2D) planar structures. To improve the electrocatalytic HER efficiency, it is crucial to effectively increase the surface area for catalyst loading. Hence, the research into three-dimensional (3D) electrode structures is emergent. A three-dimensional graphene foam synthesized on the Ni foam skeleton by chemical vapor deposition (CVD) has been reported.[36, 37] The graphene foam without the support of an Ni skeleton is …