High aspect-ratio Li2ZrO3 nanotube (NT) layers were obtained by hydrothermal synthesis in LiOH solution using anodic ZrO2 NT arrays as templates. Characterizations of SEM, XRD, and TEM were performed. The results showed that tetragonal Li2ZrO3 NTs arrays containing a little monoclinic ZrO2 can be obtained using this simple method. The mean diameter of the NTs is approximately 150 nm. The alkalinity of hydrothermal solution was proved to have significant effect on the formation of the Li2ZrO3 NT arrays. Under different alkalinity, different growth mechanisms dominated the formation of the nanotubular layers.