Molybdenum disulfide (MoS2), as a promising catalyst, has been widely investigated for hydrogen evolution reaction (HER). But the low density and poor reactivity of active sites, poor electrical transport, and inefficient electrical contact to the catalyst, leads to the modest performance. In this work, we demonstrate an effective route to overcome those issues by decorating the conductive LixMoS2 nanoparticles on the three-dimensional carbon fiber paper (CFP) through combining hydrothermal method and lithium intercalation. Thus, the dense LixMoS2 nanoparticles of the surface can provide the large number of exposed active sites, the highly-conductive LixMoS2 nanoparticles and CFP substrate can facilitate the transfer of electron not only between the LixMoS2 nanoparticles and CFP, but also between the whole sample and current collector, and the porous networked structure can enable the diffusion and penetration of electrolyte. Prompted by those advantage, the as-prepared samples exhibit outstanding HER catalytic activity with the small Tafel slope of 62 my dec(-1) and the low overpotential of -115.6 mV vs RHE at an electrocatalytic current density of 10 mA cm(-2). Chronoamperometric current test for 10 h confirms the long-term stability of the catalyst. (C) 2016 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.