Bridging Adsorption and Catalysis Through an Entangled Mo–O/Mo–N Coordination Environment for High‐Performance Lithium–Sulfur Batteries

ABSTRACT The practical application of lithium–sulfur (Li–S) batteries is severely hindered by the intrinsically sluggish redox kinetics and uncontrolled shuttle behavior of lithium polysulfides (LiPSs), while current catalytic strategies remain limited by insufficient integration of adsorption–conversion functionalities and inefficient interfacial electron transfer. Herein, we propose a Mo–O/Mo–N entangled coordination framework by coupling atomically dispersed Mo sites with an amorphous MoO 3‐x –MoN heterojunction on conductive MXene nanosheets. This architecture enables a triple‐site synergistic mechanism, where oxygen‐deficient MoO 3‐x ensures strong chemisorption of LiPSs, MoN accelerates catalytic conversion, and Mo single atoms further optimize the interfacial electronic structure and reaction kinetics. Benefiting from the synergistic modulation of adsorption strength and catalytic activity, the designed interlayer effectively suppresses LiPSs diffusion and promotes rapid and reversible sulfur redox reactions. As a result, the Li–S batteries deliver an ultralow capacity decay of 0.019% per cycle over 1400 cycles at 1 C, along with a high areal capacity of 5.35 mAh cm −2 under practical sulfur loading. This work provides new insights into atomic‐level coordination engineering and heterointerface design for advanced Li–S batteries.