Designing defect‐rich MoS2/C architectures with three‐dimensional (3D) porous frame effectively improve the electrochemical performance of lithium‐ion batteries (LIBs) owing to the improved conductivity and decreased diffusion distance of Li+ ions for lithium storage. Herein, we report a reliable morphology engineering method combining with tunable defects to synthesize defect‐rich MoS2 nanosheets with a few layers entrapped carbon sheath, forming a 3D porous conductive network architecture. The defect‐rich MoS2 nanosheets with expanded interlayers can provide a shortened ion diffusion path, and realize the 3D Li+ diffusion with faster kinetics. A 3D conductive interconnected carbon network is able to improve interparticle conductivity, concurrently maintaining the structural integrity. Benefiting from these intriguing features, the as‐prepared MoS2/C architectures exhibit excellent electrochemical performance: a high reversible capacity of 1163 mAh g−1 at a current density of 0.1 A g−1 after 100 cycles and a high rate capability of 800 mAh g−1 at 5 A g−1. Defect content in MoS2/C architectures can be obtained by changing H2 concentration. Compared with the counterparts with few defects, the defect‐rich MoS2/C architectures show improved electrochemical stability with a superior cycle life, illustrating a highly reversible capacity of 751 mAh g−1 at 0.5 A g−1 after 500 cycles.
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