A facile one-step spraying synthesis of MoS2/C microspheres and their enhanced electrochemical performance as anode of sodium-ion batteries is reported. An aerosol spraying pyrolysis without any template is employed to synthesize MoS2/C microspheres, in which ultrathin MoS2 nanosheets (approximate to 2 nm) with enlarged interlayers (approximate to 0.64 nm) are homogeneously embedded in mesoporous carbon microspheres. The as-synthesized mesoporous MoS2/C microspheres with 31 wt% carbon have been applied as an anode material for sodium ion batteries, demonstrating long cycling stability (390 mAh g(-1) after 2500 cycles at 1.0 A g(-1)) and high rate capability (312 mAh g(-1) at 10.0 A g(-1) and 244 mAh g(-1) at 20.0 A g(-1)). The superior electrochemical performance is due to the uniform distribution of ultrathin MoS2 nanosheets in mesoporous carbon frameworks. This kind of structure not only effectively improves the electronic and ionic transport through MoS2/C microspheres, but also minimizes the influence of pulverization and aggregation of MoS2 nanosheets during repeated sodiation and desodiation.