Mechanochemical-hydrothermal synthesis is a low-cost and efficient method to prepare functional particles, due to the local high-pressure and high-temperature reaction fields generated during the process. Here, mechanochemical-hydrothermal synthesis of layered lithium titanate hydrate, Li1.81H0.19Ti2O5·xH2O (LHTO), using a planetary ball mill is demonstrated. By planetary ball milling of LiOH and TiO2 with water at room temperature, LHTO nanotubes with lengths over 300nm were synthesized. The synthesized LHTO nanotubes were transformed to Li4Ti5O12 (LTO), which is a common anode material for Li-ion batteries, via thermal treatment while maintaining the nanotube morphology. The anode properties of the thermally prepared LTO nanotubes exhibited a first discharge capacity of 160mAh/g at a rate of 0.1C, even though residual TiO2 and contamination from ZrO2 milling balls were observed as product impurities. The reduction of impurities in the product after mechanochemical-hydrothermal synthesis is important to improve material performances.