Lithium-ion batteries with green and inexpensive aqueous electrolytes solve the safety problem associated with conventional lithium-ion batteries that use highly toxic and flammable organic solvents, which usually cause fires and explosions. However, the relatively low capacities (usually <65 mAh g(-1)) and less than 50% capacity retention over 50 cycles unfortunately limit their promising applicability. Herein, a novel model of ordered lamellar organic-inorganic hybrid nanorods is first put forward as an excellent platform to circumvent the above issues. Taking the synthetic highly ordered lamellar V2O3-based hybrid nanorods as an example, they deliver a capacity up to 131 mAh g(-1), nearly 1.5 and 2 times higher than that of 10-nm V2O3 nanocrystals (90 mAh g(-1)) and 2-mu m bulk V2O3 (73.9 mAhg(-1)). Also, their excellent cyclability of 88% after 50 cycles is remarkably better than that of 10-nm V2O3 nanocrystals (64%) and 2-mu m bulk V2O3 (41%). This work provides a facile route for gram-scale synthesizing highly ordered lamellar hybrid materials and proves that these unique structures are excellent platforms for significantly improving aqueous lithium-ion battery performances especially at high discharge rates, giving tantalizing perspectives in future design and synthesis of high-performance active materials for aqueous lithium-ion batteries. (C) 2011 Elsevier B.V. All rights reserved.