Buried aluminum/polymer interfaces were studied using a spectroelectrochemical experimental setup based on simultaneous in situ attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR) and electrical impedance spectroscopy (EIS). Transport of water and electrolyte through the polymer film to the aluminum/polymer interface and oxidation/corrosion of aluminum was followed by ATR-FTIR, while the impedance behavior of the system was simultaneously studied by EIS. As the ATR-FTIR technique is specific for the aluminum/polymer interfacial region while EIS takes into account alterations of both the polymer bulk and the interface, the combined setup provides complementary information of the system investigated. (c) 2007 The Electrochemical Society.