A custom separator with an ultra-lightweight polyaniline nanofibers/multiwall carbon nanotubes (PANiNF/MWCNT) coating has been utilized in lithium-sulfur (Li-S) battery for investigating the electrochemical performance of a hybrid conductive-polymer/carbon coating.The cells employing the PANiNF/MWCNT-functionalized separators facilitate high reversible capacities of 709, 641, and 612 mA h g -1 at, respectively, C/5, C/2, and 1C rates after 100 cycles.High charge-storage capacity retention was also found in the cell with the PANiNF/MWCNTfunctionalized separator after a resting time of 12 h. Such dynamically and statically electrochemical stability could be ascribed to the synergistic physical adsorption and chemical immobilization of the polysulfides by the ultra-lightweight PANiNF/MWCNT coating (only 0.01 mg cm -2 ). This demonstrates that the design of hybrid polymer/carbon-coated-separators has the potential to become a viable approach for successfully developing practical Li-S batteries. 7 contrast, cells employing the bare Celgard separator have poor R QH and R QL (Q H : 78 %, R QH: 31 %; Q L 40 %; R QL 37 %) after only 50 cycles (Fig. S5d in ESI).The comparative analysis between the two functionalized separators shows that the MWCNT-functionalized separator has the higher discharge capacity during the initial several cycles since the use of sp 2 carbon network alone can assist fast electron transport (Fig. 4a). 7Nevertheless, the capacities fade relatively fast due to the easy detachment of polysulfides from the ultra-lightweight MWCNT layer during the discharge process. [10][11][12] In contrast, the PANiNF/MWCNT-functionalized separator displays excellent capacity utilization and retention at various cycling rates during long cycles in spite of the extremely lightweight functional layer. This is because the PANiNF/MWCNT coating possesses (i) the hybrid conductive PANiNF/MWCNT network to guarantee the high redox accessibility and (ii) the functional groups to strengthen the chemical polysulfide-immobilizing capability. [10][11][12] The strong interaction between the PANi and sulfur-containing species for the improved cycle stability is much debated in the literature. [10][11][12][14][15][16] Subsequently, the hybrid polymer/carbon coating may allow reducing the weight of the coating layer immensely, yet retain the stable cyclability. This finding is supported by the enhanced cycle stability of the cells employing the ultra-lightweight PANiNF/MWCNT-functionalized separators, which exhibit a high reversible discharge capacity of 709 mA h g -1 after 100 cycles. The corresponding capacity retention rate and capacity fade rate approach, respectively, 70 % and 0.3 % per cycle. As a reference, the capacity fade rates of the reference cells using the MWCNT-functionalized separator and the Celgard separator are, respectively, 1.29 % per cycle and 1.31 % per cycle after 50 cycles.The rate performance of the PANiNF/MWCNT-functionalized separator is shown in Fig. 4a. The initial discharge capacities approach 1020, 867...