Methods of fabricating semiconductor devices are provided. The method includes forming an interconnect structure over a substrate. The method also includes forming a passivation layer over the interconnect structure. The method further includes forming an opening in the passivation layer to expose a portion of the interconnect structure. In addition, the method includes sequentially forming a lower barrier film, an upper barrier film, and an aluminum-containing layer in the opening. The lower barrier film and the upper barrier film are made of metal nitride, and the upper barrier film has a nitrogen atomic percentage that is higher than a nitrogen atomic percentage of the lower barrier film and has an amorphous structure.