A novel, high-yield, one-step approach was developed to prepare MoS2/graphene nanosheets (GNS) by exfoliating commercial bulk MoS2 and graphite via solid-state pan-milling. We found that pan-milling could be used to co-exfoliate MoS2 and graphite into few-layer MoS2/GNS heterostructures, which could improve the electronic conductivity between the MoS2 layers and could decrease the Li+ diffusion barrier at the MoS2/graphene interfaces. As an anode material in lithium-ion batteries (LIBs), the MoS2/GNS milled for 10 cycles, exhibited a high reversible capacity of about 654 mAh g(-1) after 150 cycles at 200 mA g(-1), and had excellent rate capability (418 mAh g(-1) at 2 A g(-1)) compared to commercial MoS2/graphite. The method described in this work provides a simple and ecofriendly strategy for the preparation of two-dimensional materials and composites by exfoliating commercial crystalline materials.