Compact and uniform layered double hydroxides thin films were fabricated on aluminum substrates using a simple solution-immersion process; upon chemical modification with perfluorosilane, the wettability of the aluminum surface changed from hydrophilic to superhydrophobic. The products were characterized by scanning electron microscopy, X-ray powder diffraction, and X-ray photoelectron spectroscopy. It is confirmed that the synergic effect of the surface morphology and the surface free energy contribute to this unique surface water repellence. In addition, the superhydrophobic films possess long-term storage stability and good adhesion strength to aluminum substrates, which enhance their potential practical applications.