Ultrathin nanosheets made by transition metal dichalcogenide show the potential as high-capacity anode materials for lithium ion batteries (LIBs). However, the tendency of restacking individual nanosheet due to strong van der Waals force, a dramatic volume variation upon continuous cycling, as well as poor intrinsic conductivity greatly restrict their practical applications. In this work, high content metallic phase molybdenum disulfide (1T/2H–MoS2) ultrathin nanosheets with higher intrinsic conductivity and extended interlayer distance are vertically assembled on the outer surface of chemically activated hollow carbon nanospheres (CAHCSs) through a facile solvothermal method. Phase structure, chemical composition, and microstructure studies show that the obtained composites (CAHCSs@1T/2H–MoS2) have optimized structural and compositional advantages to efficiently store lithium ions. When evaluated as anodes for LIBs, the CAHCSs@1T/2H–MoS2 electrode show excellent fast and stable lithium storage properties. In specific, the CAHCSs@1T/2H–MoS2 electrode delivers a large reversible capacity of 831 mAh g−1 at 1 A g−1 after 200 cycles. At a higher current density of 2 A g−1, the CAHCSs@1T/2H–MoS2 electrode has a reversible capacity of 863 mAh g−1. The proposed electrode design strategy provides an alternative route to promote the ion storage in transition-metal-dichalcogenides-based materials.