The shuttle effect, which causes the loss of active sulfur, passivation of lithium anode, and leads to severe capacity attenuation, is currently the main bottleneck for lithium-sulfur batteries. Recent studies have disclosed that molybdenum compounds possess exceptional advantages as a polar substrate to immobilize and catalyze lithium polysulfide such as high conductivity and strong sulfiphilicity. However, these materials show incomplete contact with sulfur/polysulfides, which causes uneven redox conversion of sulfur and results in poor rate performance. Herein, a new type of 2D nano-channeled molybdenum compounds (2D-MoN x ) via the 2D organic-polyoxometalate superstructure for accelerating interfacial polysulfide catalysis toward high-performance lithium-sulfur batteries is reported. The 2D-MoN x shows well-interlinked nano-channels, which increase the reactive interface and contact surface with polysulfides. Therefore, the battery equipped with 2D-MoN x displays a high discharge capacity of 912.7 mAh g -1 at 1 C and the highest capacity retention of 523.7 mAh g -1 after 300 cycles. Even at the rate of 2 C, the capacity retention can be maintained at 526.6 mAh g -1 after 300 cycles. This innovative nano-channel and interfacial design of 2D-MoN x provides new nanostructures to optimize the sulfur redox chemistry and eliminate the shuttle effect of polysulfides.