Iron disulfide (FeS 2 ), a low-cost material, displays considerable theoretical specific capacity (894 mA h g −1 ) but still suffers from shuttling of polysulfides and sluggish kinetics. The MoO 2 electrocatalyst has been successfully applied in Li−S systems, bringing about fascinated electrochemical improvements. Herein, through the gasification coating manners, the ultra-uniform distribution of MoO 2 with abundant catalytic sites is surprisingly obtained, incorporating with the establishment of interfacial Fe− O−Mo bonds. Benefiting from the unique structural traits, optimized FeS 2 @MoO 2 delivers an initial discharge capacity of 1271 mA h g −1 . In addition, after 100 cycles, the capacity of FeS 2 @ MoO 2 could reach ∼308 mA h g −1 , larger than that of pristine FeS 2 . Supported by the kinetic analysis, it could be found that the existing Fe−O−Mo bonds contribute to enhanced ion/e − diffusion behaviors during the intercalation/deintercalation process, ultimately resulting in outstanding lithium-ion storage capacity. Moreover, benefitting from the detailed resistance analysis and the galvanostatic intermittent titration technique test, the existence of MoO 2 and Fe−O−Mo interfacial bonds could facilitate the diffusion of ions/electrons transferring and structural stability. Thus, this work is expected to provide insights into the construction of MoO 2 ultra-uniformly coated FeS 2 with tailored interfacial traits in energy storage systems.