The Cr2O3 with high-energy density and relatively low lithium insertion potential is a promising anode candidate for LIBs. However, the intrinsic poor electroconductivity and side effects like volume expansion of Cr2O3 severely limit its capacity and cyclability at high charge/discharge rates. To address the problem, the amorphous Cr2O3/N-doped carbon nanosheets (denoted as a-Cr2O3/NC) have been designed and prepared by an easy one-step solution combustion synthesis method from a uniform solution of chromium nitrate, glucose, and glycine. The as-synthesized a-Cr2O3/NC consist of amorphous Cr2O3 particles and N-doped carbon sheet, where the amorphous Cr2O3 is evenly encapsulated in the carbon sheet support. An anode prepared from the synthesized a-Cr2O3/NC demonstrates much higher specific capacity and better cycling performance than the crystalline Cr2O3 anode. Upon extended cycling, the a-Cr2O3/NC anode exhibits good long-term stability and its reversible capacity retains as high as 782.4 mAh g(-1) after 500 cycles at 1 A g(-1). Such good performance stems from its unique structure. The amorphous structure of Cr2O3 can furnish a mass of enterable active sites which can favor the lithium ions insertion/extraction, whereas the sheet-like N-doped carbon support can increase the electroconductivity and facilitate the transportation of lithium ions and electrons.