Lithium-sulfur (Li-S) batteries hold great promise for new-generation energy storage technologies owing to their overwhelming energy density. However, the poor conductivity of active sulfur and the shuttle effect limit their widespread use. Herein, a carbon cloth decorated with thiol-containing UiO-66 nanoparticles (CC@UiO-66(SH) 2 ) was developed to substitute the traditional interlayer and current collector for Li-S batteries. One side of CC@UiO-66(SH) 2 acts as a current collector to load active materials, while the other side serves as an interlayer to further restrain polysulfide shuttling. This two-in-one integrated architecture endows the sulfur cathode with fast electron/ion transport and efficient chemical confinement of polysulfides. More importantly, rich thiol groups in the pores of UiO-66(SH) 2 serve to tether polysulfides by both covalent interactions and lithium bonding. Therefore, the Li-S battery equipped with this integrated interlayer-current collector not only delivers an enhanced specific capability (1209 mAh g -1 at 0.1 C) but also exhibits prominent cycling stability (an attenuation rate of 0.037% per cycle for 1000 cycles at 1 C). Meanwhile, the battery achieves a high discharge capacity of 795 mAh g -1 at a sulfur loading of 3.83 mg cm -2 . The new metal-organic framework (MOF)-based electrode material reported in this study undoubtedly provides insights into the exploration of functional MOFs for robust Li-S batteries.