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Sulfur-polyacrylonitrile (S-PAN) composite has been developed as a novel composite cathode material to address many issues with conventional Li-S batteries (LSBs). In this study, a freestanding S-PAN-CNT composite is first developed as the cathode material for LSBs, which is capable to deliver a high specific capacity of 1458 mAh g-1 at 0.2C and a desirable high-rate performance of 1097 mAh g-1 at 2.0 C. Furthermore, a Li2S-PAN-CNT cathode is obtained via in-situ direct pre-lithiation of S-PAN-CNT composite, which exhibits an even improved discharge capacity, cycling performance, and rate capability. Lastly, we develop Li-ion sulfur full batteries based on both S-PAN-CNT and Li2S-PAN-CNT cathode. The excellent electrochemical performance and corresponding theoretical estimation both demonstrate that the proposed system as a promising metal-free Li-ion battery with a high specific capacity, good cycle life, and low cost.