their high energy density and long cycle life. Intensive studies have been focused on improving LIBs in the aspects of power and energy density, cycling lifetime, safety characteristics, and cost, in order to fulfill the ever-increasing demand of EVs and HEVs. [1,2] However, the state-of-the-art LIBs are still insufficient enough to meet the strict standard of future EVs in terms of power output and driving distance. It is expected that the desired improvements on LIBs can be achieved by engineering novel architectures on current electrode materials and developing all-solid-state batteries.TiO 2 has been studied extensively as an anode material for LIBs, since it is stable, environmentally benign, and of low fabrication cost. It also delivers a high Li-insertion potential (≈1.7 V versus Li/Li + ) and has a rather low self-discharge rate. [3][4][5][6] Considering electrochemical performance of different polymorphs of TiO 2 , anatase TiO 2 is remarkable of its reversible uptake of 0.5 Li per formula unit, leading to a theoretical charge storage capacity of 167.5 mA h g −1 . [3,4] However, TiO 2 suffers from poor electronic conductivity and slow lithium-ion diffusion kinetics. The Li + ion diffusion coefficient in anatase TiO 2 is ≈10 −13 -10 −17 cm 2 s −1 . The electronic conductivity of anatase is also low at ≈10 −12 S cm −1 . [7] The problems can be addressed from two perspectives. First, TiO 2 can be combined with highly conductive materials, such as carbon nanotubes (CNTs) and graphene. [8][9][10] To further boost the electrochemical performance, a Li + ion conductive material can be applied to help facilitate ion transport. Li et al. reported improved battery performance by coating the electrode material with solid-state electrolyte. [11] The second approach to solving the problems is nanostructuring. The downsizing dimensions not only significantly reduce the ionic and electronic diffusion length but also provide a high surface area, giving high rate and cycling performances. [12] Atomic layer deposition (ALD) is a gas-phase deposition technique and capable to uniformly deposit ultrathin TiO 2 on materials of high aspect ratios. ALD is featured by two sequentially cyclic self-limiting reactions. The saturated surface reactions allow the film to grow layer-by-layer, Atomic layer deposition (ALD) is considered as a powerful technique to synthesize novel electrode materials for lithium-ion batteries (LIBs), because not only the compositions can be specifically designed to achieve higher battery performances, but also the materials can be deposited on various substrates for different purposes. Herein, a novel design of active material/ electrolyte mixture electrode, i.e., titanium dioxide/lithium phosphate (TLPO) nanocomposite, has been successfully developed by ALD and deposited on carbon nanotube substrates (CNTs@TLPO) at 250 °C, by combining the ALD recipes of TiO 2 and lithium phosphate (LPO). In the nanocomposite, TiO 2 forms anatase nanocrystals, embedded in a matrix of amorphous lithium phosphate. CNTs@TLP...