| Summary: | Abstract Lithium‐sulfur (Li‐S) batteries are considered as one of the most promising energy storage systems for next‐generation electric vehicles because of their high‐energy density. However, the poor cyclic stability, especially at a high sulfur loading, is the major obstacles retarding their practical use. Inspired by the nacre structure of an abalone, a similar configuration consisting of layered carbon nanotube (CNT) matrix and compactly embedded sulfur is designed as the cathode for Li‐S batteries, which are realized by a well‐designed unidirectional freeze‐drying approach. The compact and lamellar configuration with closely contacted neighboring CNT layers and the strong interaction between the highly conductive network and polysulfides have realized a high sulfur loading with significantly restrained polysulfide shuttling, resulting in a superior cyclic stability and an excellent rate performance for the produced Li‐S batteries. Typically, with a sulfur loading of 5 mg cm−2, the assembled batteries demonstrate discharge capacities of 1236 mAh g−1 at 0.1 C, 498 mAh g−1 at 2 C and moreover, when the sulfur loading is further increased to 10 mg cm−2 coupling with a carbon‐coated separator, a superhigh areal capacity of 11.0 mAh cm−2 is achieved.
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