The study of liquid crystal (LC) alignment is important for fundamental researches and industrial applications. The tunable pretilt angles of liquid crystal (LC) molecules aligned on the inorganic zinc oxide (ZnO) nanostructure films with controllable surface wettability are demonstrated in this work. The ZnO nanostructure films are deposited on the ITO- glass substrates by the two-steps hydrothermal process, and their wettability can be modified by annealing. Our experimental results show that the pretilt angles of LCs on ZnO nanostructure films can be successfully adjusted over a wide range from ∼90° to ∼0° as the surface energy on the ZnO nanostructure films changes from ∼30 to ∼70 mJ/m. Finally we have applied this technique to fabricate a no-bias optically-compensated bend (OCB) LCD with ZnO nanostructure films annealed at 235 °C.