In this work, thin ALD alumina films were fabricated for evaluating their capabilities as a barrier material for corrosive environments. The fracture toughness and the corrosion-resisting properties after fatigue cycle of these thin ALD alumina films have been characterized. Indentation tests indicate that the ALD alumina/Al structures could enhance both the yield strength of the metal and the effective fracture toughness of the coated ALD alumina films and this result could be useful for designing nanocomposite structures. However, the test results also indicate that the interfacial strength of the ALD/Al structures was prone to degrade under fatigue loading under corrosive environment. This could potentially be a problem for the long term reliability of related devices operated under a harsh environment. In addition, the strong correlation between indentation behavior and fatigue loading for the structure indicate that nanoindentation response could be possibly used to indicate the damage level of microstructures for future reliability evaluations.