2H-MoS2 is a well-studied and promising non-noble metal electrocatalyst for heterogeneous reactions,such as the hydrogen evolution reaction(HER).The performance is largely limited by the chemically inert basal plane,which is unfavorable for surface adsorption and reactions.Herein,we report a facile method to boost the HER activities of 2H-MoS2 by coupling with epitaxial Bi2Te3 topological insulator films.The as-obtained MoS2/Bi2Te3/SrTiO3 catalyst exhibits prominent HER catalytic activities compared to that of pure MoS2 structures,with a 189 mV decrease in the overpotential required to reach a current density of 10 mA cm-2 and a low Tafel slope of 58 mV dec-1.Theoretical investigations suggest that the enhanced catalytic activity originates from the charge redistribution at the interface between the Bi2Te3topological insulator films and the MoS2 layer.The delocalized sp-derived topological surface states could denote electrons to the MoS2 layer and activate the basal plane for hydrogen adsorption.This study demon-strates the potential of manipulating topological surface states to design high-performance electrocatalysts.