Superlattices are rising stars on the horizon of energy storage and conversion, bringing new functionalities; however, their complex synthesis limits their large‐scale production and application. Herein, a simple solution‐based method is reported to produce organic–inorganic superlattices and demonstrate that the pyrolysis of the organic compound enables tuning their interlayer space. This strategy is exemplified here by combining polyvinyl pyrrolidone (PVP) with WSe2 within PVP/WSe2 superlattices. The annealing of such heterostructures results in N‐doped graphene/WSe2 (NG/WSe2) superlattices with a continuously adjustable interlayer space in the range from 10.4 to 21 Å. Such NG/WSe2 superlattices show a metallic electronic character with outstanding electrical conductivities. Both experimental results and theoretical calculations further demonstrate that these superlattices are excellent sulfur hosts at the cathode of lithium–sulfur batteries (LSB), being able to effectively reduce the lithium polysulfide shuttle effect by dual‐adsorption sites and accelerating the sluggish Li–S reaction kinetics. Consequently, S@NG/WSe2 electrodes enable LSBs characterized by high sulfur usages, superior rate performance, and outstanding cycling stability, even at high sulfur loadings, lean electrolyte conditions, and at the pouch cell level. Overall, this work not only establishes a cost‐effective strategy to produce artificial superlattice materials but also pioneers their application in the field of LSBs.

Developing high-performance cathode host materials is fundamental to solve the low utilization of sulfur, the sluggish redox kinetics, and the lithium polysulfide (LiPS) shuttle effect in lithium–sulfur batteries (LSBs). Here, a multifunctional Ag/VN@Co/NCNT nanocomposite with multiple adsorption and catalytic sites within hierarchical nanoreactors is reported as a robust sulfur host for LSB cathodes. In this hierarchical nanoreactor, heterostructured Ag/VN nanorods serve as a highly conductive backbone structure and provide internal catalytic and adsorption sites for LiPS conversion. Interconnected nitrogen-doped carbon nanotubes (NCNTs), in situ grown from the Ag/VN surface, greatly improve the overall specific surface area for sulfur dispersion and accommodate volume changes in the reaction process. Owing to their high LiPS adsorption ability, outer Co nanoparticles at the top of the NCNTs catch escaped LiPS, thus effectively suppressing the shuttle effect and enhancing kinetics. Benefiting from the multiple adsorption and catalytic sites of the developed hierarchical nanoreactors, Ag/VN@Co/NCNTs@S cathodes display outstanding electrochemical performances, including a superior rate performance of 609.7 mAh g–1 at 4 C and a good stability with a capacity decay of 0.018% per cycle after 2000 cycles at 2 C. These properties demonstrate the exceptional potential of Ag/VN@Co/NCNTs@S nanocomposites and approach LSBs closer to their real-world application.

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