The rechargeable lithium–sulfur battery is a promising option for energy storage applications because of its low cost and high energy density. The electrochemical performance of the sulfur cathode, however, is substantially compromised because of fast capacity decay caused by polysulfide dissolution/shuttling and low specific capacity caused by the poor electrical conductivities of the active materials. Herein we demonstrate a novel strategy to address these two problems by designing and synthesizing a carbon nanotube (CNT)/NiFe<sub>2</sub>O<sub>4</sub>–S ternary hybrid material structure. In this unique material architecture, each component synergistically serves a specific purpose: The porous CNT network provides fast electron conduction paths and structural stability. The NiFe<sub>2</sub>O<sub>4</sub> nanosheets afford strong binding sites for trapping polysulfide intermediates. The fine S nanoparticles well-distributed on the CNT/NiFe<sub>2</sub>O<sub>4</sub> scaffold facilitate fast Li<sup>+</sup> storage and release for energy delivery. The hybrid material exhibits balanced high performance with respect to specific capacity, rate capability, and cycling stability with outstandingly high Coulombic efficiency. Reversible specific capacities of 1350 and 900 mAh g<sup>–1</sup> are achieved at rates of 0.1 and 1 C respectively, together with an unprecedented cycling stability of ∼0.009% capacity decay per cycle over more than 500 cycles
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