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Molybdenum disulfide (MoS 2) is one of the promising candidates for hydrogen evolution reaction (HER), it's HER properties can be extremely enhanced by the construction of nanostructure and the regulation of electronic structure. In this paper, hierarchical composites with MoS 2 and carbon nanotubes (CNTs) as the noble metal-free electrocatalysts for HER were fabricated through calcination and hydrothermal processes, in which the MoS 2 nanosheets with Ni atoms incorporation were vertically grown on the outsides of nitrogen (N)-doped CNTs. The constructed hierarchical structures provide large specific surface area of about 150 m2 g−1 and high structure stability. Importantly, the MoS 2 nanosheets with enlarged interlayer spacing possess ultrathin structure of about 4 nm in thickness. Owing to the incorporation of Ni atoms, abundant unsaturated S atoms are obtained in the basal plane, which leading to more active sites exposed during HER processes. Meanwhile, N-doped CNTs can act as the substrate for MoS 2 nanosheets growing and simultaneously improve the conductivity of catalyst. Based on the synergy of hierarchical structure, increased active sites and enhanced conductivity, the as-prepared electrocatalysts exhibit superior HER activity with low overpotentials, small Tafel slopes and long-time durability in both acidic and alkaline electrolytes. The overpotentials of 158 and 179 mV were required to drive HER current density up to 10 mA cm−2 in 0.5 M H 2 SO 4 and 1.0 M KOH, respectively. This work reports a highly efficient MoS 2 -based electrocatalyst for HER via fabricating hierarchical structure and doping Ni atoms. Image 1 [ABSTRACT FROM AUTHOR]