Integrated Design of Interlayer/Current‐Collector: Heteronanowires Decorated Carbon Microtube Fabric for High‐Loading and Lean‐Electrolyte Lithium–Sulfur Batteries

Abstract Low sulfur loading, high electrolyte/sulfur (E/S) ratio, and sluggish sulfur redox reaction are the main challenges that severely impede the practical application of lithium–sulfur batteries (LSBs). To address these problems, a self‐standing hollow carbonized cotton cloth (CCC) decorated with TiO 2 ‐TiN heteronanowires (CCC@TiO 2 ‐TiN) is proposed to replace the traditional cathode. Concretely, one side of CCC@TiO 2 ‐TiN serves as a current‐collector to load sulfur (CCC@TiO 2 ‐TiN/S), while the other side facing the separator acts as interlayer to inhibit shuttle effect. This advanced intergrated interlayer/current‐collector cathode is endowed with excellent 3D electron/ion transportation, a strong confinement barrier, and vast sulfur loading sites. Moreover, the as‐developed TiO 2 ‐TiN heteronanowires work as in situ capture and catalysis sites for the reversible and accelerated sulfur redox reaction. Therefore, the intergrated cathode of CCC@TiO 2 ‐TiN/S achieves an ultrahigh sulfur loading of 13 mg cm −2 and delivers a superb areal capacity of 9.09 mAh cm −2 under the ultralow E/S ratio of 4.6 µL mg −1 . This work provides a new model material to achieve high sulfur loading and lean‐electrolyte toward the practical LSBs with high specific energy density.