We have employed plasma-enhanced and thermal atomic layer deposition (ALD) within the temperature range of 50-150 degrees C for the deposition of ultra-thin (10-50 nm) Al2O3 films on 100Cr6 steel and aluminium Al2024-T3 alloys. [Al(CH3)(3)] was used as the precursor with either an O-2 plasma or water as co-reactants. Neutral salt spray tests showed that the thicker films offered the best corrosion-resistance. Using cyclic voltametry, the 50 nm films were found to be the least porous (< 0.5%). For 10 nm thick films, plasma-enhanced ALD afforded a lower porosity and higher film density than thermal ALD. ToF-SIMS measurements on 100Cr6 showed that the main 'bulk' of the films contained very few impurities, but OH and C were observed at the interfaces. TEM confirmed that the films were conformal on all substrates and the adhesion was excellent for the films deposited by plasma-enhanced ALD but not for thermal ALD, as delamination was observed. On the basis of these and other results, the prospects of the application of ALD films for corrosion protection, and the use of plasma-enhanced ALD to promote their nucleation, is discussed. (C) 2011 The Electrochemical Society. [DOI: 10.1149/1.3560197] All rights reserved.