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Interface engineering has been widely explored to improve the electrochemical performances of composite electrodes, which governs the interface charge transfer, electron transportation, and structural stability. Herein, MoC is incorporated into -MoSe2/C compos?ite as an intermediate phase to alter the bridging between -MoSe2- and nitrogen-doped three-dimensional (3D) carbon framework as -MoSe2/MoC/N–C connection, which greatly improve the structural stability, electronic conductivity, and interfacial charge transfer. Moreover, theincorporation of MoC into the composites inhibits the overgrowth of -MoSe2 nanosheets on the 3D carbon framework, producing much smaller -MoSe2 nanodots. The obtained -MoSe2 nanodots with fewer layers, rich edge sites, and heteroatom doping ensure the good kinetics to promote pseudo-capacitance contributions. Employing as anode material for lithium-ion batteries, it shows ultralong cycle life (with 90% capacity retention after 5000 cycles at 2 A g?1) and excellent rate capability. Moreover, the constructed -LiFePO4//MoSe2/MoC/N–C full cell exhibits over 86% capacity retention at 2 A g?1 after 300 cycles. The results demonstrate the effectiveness of the interface engineering by incorporation of MoC as interface bridging intermediate to boost the lithium storage capability, which can be extended as a potential general strategy for the interface engineering of composite materials.