The carbon-coated chevrel phase of Mo6S8 as electrode material was fabricated for the first time. Compared with the bare Mo6S8 and 10%C-Mo6S8 anodes, the 5%C-Mo6S8 anode possesses excellent rate capability and cyclic performance at the cutoff voltage of 1.5V using LiMn2O4 as the cathode, which delivers a reversible capacity of∼85 mAh·g−1 and an average discharge voltage of as high as ∼2V maintains 93% of initial discharge capacity even after 400 cycles at 1C and in 21M aqueous electrolyte. This study provides a promising anode material for aqueous lithium-ion batteries because of its high capacity, stability and environmental inertness. Furthermore, the results demonstrate that this method could expand the synthesis and application of these unique compounds.