Crystallinity structure plays a key role in the rate capability and cycling performance for rechargeable battery. However, the effect of crystallinity structure on sodium storage properties of VS2 hasn't been clearly elucidated. In this work, VS2 nanoarchitectures comprised of the nanosheets with single-crystal or polycrystalline structure are respectively synthesized by a facile solvothermal method, and the influence of crystallinity structure on their sodium storage properties is revealed. It is found that the single-crystal structure can largely enhance the Na+ intercalation kinetics in the crystal lattice and the structure stability during charge/discharge process. Therefore, the single-crystal VS2 electrode exhibits an enhanced rate capability and cycling performance, delivering a high capacity of 193 and 172 mAhg−1 at a high rate of 0.5 and 1.0 Ag−1, and 403 mAhg−1 after the following cycling test of 200 cycles at 0.2 Ag−1. This work opens up new insights for the exploration and design of high-performance electrode materials for sodium-ion batteries.