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[en] Highlights: • Both graphene incorporation and defect engineering are carefully controlled and characterized for the first time. • Synergistic modulations of both electron and Li-ion transport kinetics are realized in the optimized G/TiO2/C/MoS2 anode. • The optimized anodes exhibit excellent capability at high current density after long-life cycles. • This work can open up an avenue for the rational design anode materials by synergistically electronic and ionic modulations. Integrating nanostructured MoS2 with low-volume-change and high-rate-performance TiO2 backbone to construct high structure stability MoS2-TiO2 based composites has been turned out to be an effective strategy. However, the long-life cycling performance at high current density of all reported MoS2-TiO2 based composites anodes is still suffered from their relatively low electron and ion transport kinetics. In this paper, we first demonstrate the successful synergistic regulations of both electron and ion transport kinetics benefits by controllable graphene incorporation and defect engineering in MoS2-TiO2 based anodes, leading to the dramatically enhanced LIBs performance. In this optimized structure with robust structure stability, few-layer MoS2 nanosheets are tightly anchored onto the surface of graphene/ultra-thin TiO2 nanosheets (G/UT-TiO2) backbone with chemical bonds. The graphene incorporation effectively improves the overall conductivity, while the defected structure of MoS2 shell can significantly facilitate Li-ions transport kinetics. As a result, the as-prepared optimized anode exhibits excellent capability (648 mAh g−1) at high current density (1 A g−1) after long-life (400) cycles, accompanied by outstanding rate performance. This work can open up an avenue for the rational design of various anode materials for high performance LIBs by synergistically structural, electronic and ionic modulations.