Practical applications of lithium-sulfur (Li-S) batteries are hindered mainly by the low sulfur utilization and severe capacity fading derived from the polysulfide shuttling. Catalysis is an effective remedy to those problems by promoting the conversion of polysulfides to reduce their accumulation in the electrolyte, which needs the catalyst to have efficient adsorption ability to soluble polysulfides and high activity for their conversion. In this work, we have proposed a bimetallic compound of NiCo₂S₄ anchored onto sulfur-doped graphene (NCS@SG) to fabricate a catalytic interlayer for Li-S batteries. Compared to CoS, the NiCo₂S₄ demonstrated much higher catalytic activity toward sulfur reduction reaction due to its multiple anchoring and catalytic active sites derived from the coordination of the bimetallic centers. As a result, the NCS@SG interlayer dramatically improved the specific capacity, rate performance, and cyclingstability of Li-S batteries. Especially, when the areal sulfur loading of the NCS@SG battery increased to 15.3 mg·cm^–2, the high-capacity retention of 93.9 % could be achieved over 50 cycles.