The layered MoS2 nanostructures have been widely used in the electrochemical hydrogen evolution reaction (HER), but rarely applied in overall water splitting application for their ignorable oxygen evolution reaction (OER) activity. To address this issue, a novel self-standing and bifunctional electrocatalyst, consisting of Co-doped MoS2 nanosheets anchored on carbon fiber paper, has been prepared via hydrothermal method. Taking advantage of conductive substrate of carbon fiber paper, sufficient-exposed active edges of MoS2 sheets, and metallic character caused by Co-doping, our electrode exhibits high-efficient bifunctional activities for the overall water splitting in alkaline electrolyte (1 M KOH), which can produce a current density of 20 mA cm(-2) at an overpotential of 197 mV for HER and 235 mV for OER. (C) 2019 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.