ZnO thin films were grown on silicon substrates using a hydrothermal method. The XRD patterns show that all of the peaks can be attributed to the wurtzite structures of ZnO. The TC value of (002) plane and average crystal size increase first and then decrease with the increase of solution concentration. SEM and AFM results show that many dense hexagonal cylinder particles have been observed on the surface of the thin films, which grown at 0.08 and 0.10 mol/L. The surface roughness of the thin films deposited at 0.06, 0.08, 0.10, and 0.12 mol/L are 24.5, 38.3, 32.0, and 39.4 nm, respectively. Surface wettability results show that the preferential orientation along c-axis and surface roughness contribute significantly to the hydrophobicity. The reversible switching between hydrophobicity and hydrophilicity is related to the synergy of the transition of wetting model, surface crystal structure, and surface roughness.