A zinc-aluminum layered double hydroxide (ZnAl-LDH)/alumina bilayer film has been fabricated on an aluminum substrate by a one-step hydrothermal crystallization method. The LDH film was uniform and compact. XRD patterns and SEM images showed that the LDH film was highly oriented with the c-axis of the crystallites parallel to the substrate surface. The alumina layer existing between the LDH film and the substrate was formed prior to the LDH during the crystallization process. Polarization measurements showed that the bilayer film exhibited a low corrosion current density value of 10(-8) A/cm(2), which means that the LDH/alumina bilayer filth can effectively protect aluminum froth corrosion. Electrochemical impedance spectroscopy (EIS) showed that the impedance of the bilayer was 16 M Omega, meaning that the film served as a passive layer with a high charge transfer resistance. The adhesion between the film and the substrate was very strong which enhances its potential for practical application.