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Lithium-sulfur (Li-S) batteries appear to be one of the most promising energy-storage devices owing to the unparalleled theoretical specific energy, relatively inexpensive price and abundant resources. Despite these attractive features, the practical performances of sulfur cathode still remain a lot of challenges, such as the electrical insulating nature of S and Li 2 S, huge volume change during cycling, notorious shuttle effect of lithium polysulfide intermediates (LiPSs), sluggish redox kinetics and construction of thick electrodes with high sulfur loading. Here, CoFe 2 O 4 nanoparticles anchored on the carbon nanotube (CNT) paper is proposed as free-standing sulfur host to address the issues. The cross-linking CNT network can serve as conductive matrix and accommodate volume change upon cycling simultaneously. Meanwhile, the CoFe 2 O 4 nanoparticles are capable of effectively anchoring LiPSs to suppress the shuttle effect and accelerating LiPSs conversion to boost redox kinetics. Moreover, the free-standing paper electrode without any binder is conducive to constructing stable cathode with high sulfur loading. In consequence, the well-designed S/CoFe 2 O 4 /CNT paper cathodes deliver impressive electrochemical performance, demonstrating an initial discharge capacity of 755.3 mAh g−1 and remaining a high reversible capacity of 642.6 mAh g−1 after 400 cycles at 2 C with an inconspicuous decay of 0.04% per cycle. The bimetallic oxide CoFe 2 O 4 nanoparticles anchored on the carbon nanotube paper is proposed as free-standing sulfur host with enhanced polysulfide trapping and catalytic effects for advanced Li-S batteries. [Display omitted] • Binder-free host realizes high sulfur loading and energy density for Li-S battery. • CoFe 2 O 4 /CNT paper inhibits the polysulfide shuttling via strong chemical interaction. • CNT-anchored CoFe 2 O 4 catalytically promotes the polysulfide conversion kinetics. • The Li-S battery with S/CoFe 2 O 4 /CNT cathode exhibits enhanced capacity and stability. [ABSTRACT FROM AUTHOR]