Chrysanthemum-like carbon/FeS microspheres (CL-C/FeS) are prepared from a one-step solvothermal method. The morphology and structure of the CL-C/FeS are characterized by X-ray diffraction, scanning electron microscopy and high-resolution transmission electron microscope. We note that the prepared CL-C/FeS microspheres exhibit the average diameter of 15 μm and possess a sheet-on-sheet structure. FeS nanosheets are stacked on the carbon sheets to form a 2D sheet-on-sheet structure, these 2D C/FeS nanosheets are self-assembled to form a 3D chrysanthemum-like morphology. Due to the unique structure, CL-C/FeS microspheres show the excellent sodium-storage performance of 500 mAh g−1 at 0.2 A g−1 and 260 mAh g−1 at 1 A g−1, which are higher than those of most reported values. Therefore, the CL-C/FeS with appropriate structure is expected to be a competitive choice for anode materials for sodium ion batteries.