Li-rich layered Li2MoO3 (LMO) materials are one promising cathode materials for Li-ion batteries due totheir high theoretical capacity and without oxygen evolution. However, the poor electrical conductivityand air instability have limited its application as a cathode material for lithium-ion battery. To solve theseproblems, Li2MoO3/g-C3N4 composites were successfully constructed by combining the molten salt andball milling methods. Carbon nitride (g-C3N4) with an abundant nitrogen-containing carbon frameworkcontains a large number of ‘‘hole” defects and double-bonded nitrogen vacancy edges, which are favorablefor the adsorption and diffusion of Li ions. In addition, density functional theory (DFT) calculationsrevealed that a stable interface can be formed between g-C3N4 and LMO, which also leads to the improvementof the electronic conductivity and the reduction of interfacial impedance of the composite. Therefore, the electrochemical performance of the composite material is significantly improved. The dischargecapacity of GLMO-5 at a current density of 1700 mA g1 is 64.6 mAh/g, which is much greater thanthe value (29.9 mAh/g) of the original LMO sample under the same conditions. EIS further shows thatGLMO-5 has the highest discharge capacity with a DLi+ value of 1.94 1014 cm2 s1. These results indicatethat constructing LMO-based composites with a highly stable layered material containing unsaturatedfunctional groups should be an effective strategy to enhance the interfacial stability, electronicconductivity, and thus the electrochemical performances of the cathode materials.