Carbon-coated magnetite (Fe3O4/C) nanocomposites with hierarchical structure have been subjected to extensive research due to their relatively large specific surface area, extra free voids, and thus enhanced electrochemical performance for lithium-ion batteries (LIBs). In this paper, Fe3O4/C nanosheets with hierarchical structure in the form of carbon matrix supporting Fe3O4 nanocrystals have been prepared by annealing the nanosheet-like iron alkoxide precursor in N2 atmosphere. The Fe3O4/C samples are characterized with X-ray powder diffraction, Raman, scanning electron microscopy, transmission electron microscopy, N2 sorption isotherms, and thermogravimetric–differential scanning calorimetric techniques, and further evaluated in the role of anode materials for LIBs. The specific discharge capacity of Fe3O4/C nanosheets obtained by annealing the precursor in N2 at 600 °C for 3 h retains 647 and 546 mAh g−1 after 100 cycles at 100 and 200 mA g−1, respectively, exhibiting superior electrochemical performance to many other Fe3O4/C nanocomposites in previous reports. The Fe3O4/C nanosheets presented here not only enrich the nanomaterial community but also provide a promising candidate functioning as an anode material for effective lithium-ion storage.