The ratio between the components determines the capacity of MoS2/carbon materials in lithium-ion batteries (LIB). However, the structure of the carbon component and the synthesis conditions determine the amount of MoS2 that can be efficiently used in each particular case. We study the influence of components ratio in MoS2/multilayer holey graphene (HG) materials on the capacity in LIB. The synthesis was carried out by hot pressing of MoS3 and HG mixtures at 600 °C and 100 bar. These synthesis conditions resulted in the decomposition of MoS3 with the formation of MoS2 nanocrystals. Optimal component distribution and better cycling performance, reaching 591 mAh g−1 at a current density of 0.1 A g−1 and 408 mAh g−1 at 1 A g−1, were found for MoS2/HG containing 30 wt.% of MoS2. An increase of the MoS2 ratio led to a decrease of cycling stability and capacity of the material.