Nanomaterials in architecture for green energy conversion and/ or storage provide one of the most desirable approaches to alleviate environmental and energy issues. [1][2][3][4] As a result, there is increasing interest in developing high-power anode materials, which can match with the state-of-the-art high-power cathode materials, for next generation high-performance rechargeable Li-ion batteries. [5][6][7] Titanium dioxide is regarded as one of the ideal candidates for high-rate anode materials, owing not only to its structural characteristics and special surface activity, [8][9][10][11] but also to its low cost, safety, and environmental benignity. The lack of open channels in bulk TiO 2 is the main drawback that restricts its capacity and rate capability for reversible lithium insertion and extraction. A reduction in the effective size and construction of open channels in the material are the main strategies currently employed to increase the rate performance. [ 1 , 4 ] The capacity could also be improved by reducing the path length of lithium ion migration and improving electron transport at the surface or in the bulk of the material. [ 10 , 12,13 ] With these strategies, the capacity of ultrafi ne TiO 2 nanocrystals and nanotubes, for example, is signifi cantly enhanced at lower rates. However, their capacity and cycle life deteriorate dramatically at higher rates. [ 9 , 14-17 ] In this respect, signifi cant efforts have recently been made on the fabrication of anatase TiO 2 nanosheets with exposed highly reactive (001) facets. [ 18 -21 ] These TiO 2 nanosheets are shown to be an excellent host structure for lithium insertion and extraction due to the presence of exposed (001) facets and short path along the [001] direction for lithium ion diffusion.Although the anatase framework undergoes insignifi cant structural distortion during lithium insertion and extraction, [ 22 ] the rate of lithium diffusion is still limited by the narrow space of the host Ti-O lattice. Also, strongly caustic NaOH and corrosive HCl or HF are commonly used for the synthesis of TiO 2 nanomaterials. [ 17,18 ] Beyond these, there is still potential danger in the high-temperature and high-pressure process in low boiling point infl ammable solvents. [ 21 ] Therefore, it is highly desirable but challenging to synthesize novel TiO 2 nanostructures as high-rate anode materials through a facile and green route. As an important group of solvents, ionic liquids (ILs), which exhibit unique properties including low volatility, a wide liquid temperature range, good dissolving ability, and designability, have been intensively used in organic synthesis, catalysis, and inorganic nanomaterials synthesis. [23][24][25][26] This inspires us to design a facile ILs-based synthetic system to prepare an attractive framework for high-effi ciency lithium storage.One such framework of TiO 2 active materials is ultrathin 2D nanosheets, which allow ultrafast surface lithium storage due to maximized Li + ion diffusion and electron transport and the elimin...