<p>Lithium-sulfur batteries (LSBs) have garnered significant attention due to their high theoretical energy density and low cost. However, the shuttle effect of polysulfides and the low conductivity of the sulfur cathode severely limit their practical application. To address these challenges, a porous carbon framework embedded with cobalt nanoparticles (Co-SPC-CTAB) is successfully prepared by calcining zeolitic imidazolate framework-67 (ZIF-67)/polypyrrole Schiff base polymer under the regulation of cetyltrimethylammonium bromide (CTAB), and it is used as the interlayer material for LSBs. The metal Co derived from ZIF-67 provides abundant adsorption-catalytic active sites, effectively facilitating the adsorption and conversion of lithium polysulfides (LiPSs). In addition, CTAB not only optimizes the pore structure of the carbon skeleton to furnish abundant channels for Li⁺ transport and electrolyte infiltration, but also helps to improve the graphitization degree of the porous carbon framework, thereby further enhancing the electrochemical energy storage kinetics of LSBs. When Co-SPC-CTAB is utilized as the interlayer material, the assembled LSBs can achieve an initial specific capacity of 1063.6 mAh g^− 1 at 1&#xa0;C and still retain 659.5 mAh g^− 1 after 500 cycles, with a capacity decay rate of only 0.076% per cycle. Under low-temperature conditions (-10&#xa0;°C), the battery can exhibit a high initial specific capacity of 931.6 mAh g^− 1 at 0.2&#xa0;C and remain at 724.8 mAh g^− 1 after 100 cycles. This study provides a novel strategy for the rational design of transition metal-carbon composite interlayer materials, advancing the development of high-stability LSBs.</p>