Lithium−sulfur batteries are considered the next generation of energy storage devices, boasting high theoretical capacity, low cost, and environmental friendliness. However, the weak conductivity of sulfur and the shuttle effect of lithium polysulfides (LiPSs) are major challenges hindering lithium−sulfur battery development. Herein, a functional interlayer composite of Fe−Co sulfide/graphene/CNTs (FCS@GC) was prepared. The composite, which benefits from the 3D cross-linked network formed by CNTs and graphene, could avoid the agglomeration effect of the carbon material and enhance the physical adsorption capacity of LiPSs, effectively improving the transfer of Li + /e − . Additionally, the loaded FeCoS 4 provides the composite with efficient chemical adsorption and conversion capacity of LiPSs, inhibits the shuttle effect at multiple levels, and greatly improves the kinetics. The lithium−sulfur battery, with FCS@GC as its functional interlayer, exhibits a stable specific capacity of 787.5 mA h g −1 after 200 charge/discharge cycles at 0.5 C. Furthermore, it showcases an initial cycling capacity of 885.5 mA h g −1 at 1 C. In addition, the capacity decay rate per cycle is only 0.036% after 800 cycles. After 110 cycles at a high sulfur loading of 5 mg cm −2 , lithium−sulfur batteries with an FCS@GC functional interlayer can still maintain a capacity of 750.5 mA h g −1 . The structure of this innovative compound will offer viable solutions for the issue of commercializing lithium−sulfur batteries.