Huge volume expansion and inferior electrical conductivity are the two main obstacles to limit the practical applications of high-capacity molybdenum disulfide (MoS) materials, which has been recognized as ideal anode materials for rechargeable lithium-ion batteries. Herein, an interfacial reinforcement structure design is proposed by conformally growing few-layered MoS nanosheets on carbon coated ultralong TiO nanotubes (TiO@C@MoS) to stabilize the solid electrolyte interface (SEI) of MoS-based electrode. The interlayer carbon coating on TiO nanotubes effectively improves the interfacial contact between MoS nanosheets and TiO nanotubes by forming Ti-O-C and C-S chemical bonds between TiO/carbon coating and MoS/carbon coating, respectively, avoiding MoS nanosheets detaching from TiO nanotubes. Meanwhile, the carbon coating serves as a buffering cushion to alleviate mechanical strain at the interface of MoS nanosheets and TiO nanotubes. Besides, it enhances the adsorption performance of Li ions on the surface of MoS and at the interface sites between MoS and TiO. While three-dimensional rigid TiO nanotubes networks work as mechanical support to suppress reaggregating and restacking of MoS nanosheets, and provide fast transportation expressways for electrons/ions. Thus, the TiO@C@MoS electrode exhibits ultrafast charge/discharge capability, a high reversible capacity of 1150 mAh g at 0.1 A g, and superior cycling performance with 90% capacity retention after 1500 cycles at 1.0 A g. This interfacial reinforcement structure design provides valuable experience to benefit rational design of alloy/conversion-typed materials electrode with high-performance.