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Molybdenum disulfide (MoS2) has been widely deemed as an attractive anode candidate for rechargeable lithium‐ion batteries (LIBs) on account of its apparently high capacity and intriguing 2‐dimensional layered structure. In our work, the growth of MoS2 nanoflowers with an expanded interlayer spacing onto nitrogen‐doped reduced graphene oxide has been successfully performed by using an effective poly(vinylpyrrolidone) (PVP)‐guided assembly route. The theoretical and experimental results indicate that PVP, as a linker, is a major contribution, both in regulating the microstructure of MoS2 nanoflowers and improving the electrochemical properties of the flower‐like MoS2/N‐graphene (F‐MoS2/NG) composite. When utilized as anode materials, the as‐made F‐MoS2/NG composite shows a boosted electrochemical performance for reversible lithium storage. It delivers a high reversible capacity of 1060 mAh/g at 100 mA/g even after 150 cycles, which is much higher than 416 mAh/g of the control MoS2/G electrode. The kinetics analysis reveals that the remarkable rate capability of F‐MoS2/NG is mainly ascribed to a pseudocapacitive process, which is rendered by its unique architecture including well‐defined MoS2 nanoflowers, the doping of nitrogen onto graphene, and the enhanced synergistic effect between them.

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