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A tube-in-tube carbon nanostructure (TTCN) with multi-walled carbon nanotubes (MWNTs) confined within hollow porous carbon nanotubes is synthesized for Li-S batteries. The structure is designed to enhance the electrical conductivity, hamper the dissolution of lithium polysulfide, and provide large pore volume for sulfur impregnation. As a cathode material for Li-S batteries, the S-TTCN composite with 71 wt% sulfur content delivers high reversible capacity, good cycling performance as well as excellent rate capabilities.