In this work, an economical route based on hydrothermal and layer-by-layer (LBL) self-assembly processes has been developed to synthesize unique Al2O3-modified LiV3O8 nanosheets, comprising a core of LiV3O8 nanosheets and a thin Al2O3 nanolayer. The thickness of the Al2O3 nanolayer can be tuned by altering the LBL cycles. When evaluated for their lithium-storage properties, the I LBL Al2O3-modified LiV3O8 nanosheets exhibit a high discharge capacity of 191 mA h g(-1) at 300 mA g(-1) (1C) over 200 cycles and excellent rate capability, demonstrating that enhanced physical and/or chemical properties can be achieved through proper surface modification. (C) 2014 Elsevier B.V. All rights reserved.