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The advent of advanced electrode materials has led to performance enhancement of traditional lithium ion batteries (LIBs). We present novel binder-free MoS coated three-dimensional carbon nanotubes (3D CNTs) as an anode in LIBs. Scanning transmission electron microscopy analysis shows that vertically oriented MoS nanoflakes are strongly bonded to CNTs, which provide a high surface area and active electrochemical sites, and enhanced ion conductivity at the interface. The electrochemical performance shows a very high areal capacity of ~1.65 mAh cm with an areal density of ~0.35 mg cm at 0.5 C rate and coulombic efficiency of ~99% up to 50 cycles. The unique architecture of 3D CNTs-MoS is indicative to be a promising anode for next generation Li-ion batteries with high capacity and long cycle life.