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Summary Lithium sulfur batteries have drawled worldwide attention in recent years, which benefit of its high‐density energetic, low cost, and environmental benignity. Nevertheless, the shuttle effect of polysulfides and resulting self‐discharge lead to capacity fade loss and poor electrochemical performance. Herein, graphitic‐carbon nitride/carbon nanotubes (g‐C3N4/CNTs) hybrid membrane is fabricated by the flow‐direct vacuum filtration process. The as‐prepared 3‐D freestanding g‐C3N4/CNTs membrane employed as positive current collector containing Li2S6 catholyte solution for lithium/polysulfides batteries. The fabricated g‐C3N4/CNTs provide a physical barriers and chemisorption resist polysulfide shuttling. Moreover, the conductive network constructed by CNTs can empower sulfur to be evenly distributed in the cathode and accelerates electron transport. Thus, to further prove the cooperative effect of g‐C3N4 and CNTs, the freestanding g‐C3N4/CNTs/Li2S6 electrode exhibits more stable electrochemical performance than CNTs/Li2S6 electrode, deliver the first discharge capacity of 876 mAh g−1 at 0.5 C and maintained at 633 mAh g−1 after 300 cycles. The sulfur mass in electrode was increased to 7.11 mg, and the g‐C3N4/CNTs/Li2S6 electrode also possess a high capacity retention of 75.5%. Meanwhile, g‐C3N4 modified CNTs can not only trap polysulfides by strong adsorption but also effectively inhibit the self‐discharge behavior of lithium/polysulfides batteries. As a consequence, the g‐C3N4/CNTs composites for lithium/polysulfides batteries are indicating an excellent electrochemical stability with a long‐term storage without obvious capacity degradation.

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