A simple electrochemical and self-assembly method was adopted for the fabrication of superhydrophobic spongelike nanostructured TiO2 surfaces with markedly controllable adhesion. Water adhesion ranging from ultralow (5.0 microN) to very high (76.6 microN) can be tuned through adjusting the nitro cellulose dosage concentrations. The detailed experiments and analyses have indicated that the significant increase of adhesion by introducing nitrocellulose is ascribed to the combination of hydrogen bonding between the nitro groups and the hydroxyl groups at the solid/liquid interfaces and the disruption of the densely packed hydrophobic 1H,1H,2H,2H-perfluorooctyltriethoxysilane (PTES) molecule. A mechanism has been proposed to explain the formation of superhydrophobic TiO2 films with distinct adhesion.