Atomic layer deposited (ALD) aluminum and tantalum oxide (Al(2)O(3) and Ta(2)O(5)) and their nanolaminates were applied as corrosion protection coatings on AISI 52100 steel. The aim was to combine the good sealing properties of Al(2)O(3) with the chemical stability of Ta(2)O(5) and to optimize the coating architecture in order to obtain the best possible long-term durability. Coating composition and morphology were studied with time-of-flight elastic recoil detection analysis (ToF-ERDA), time-of-flight secondary ion mass spectrometry (ToF-SIMS) and field emission scanning electron microscopy (FESEM) and energy dispersive x-ray spectrometry (EDS). Electrochemical properties were studied with voltammetry and electrochemical impedance spectroscopy (EIS), and corrosion durability with neutral salt spray (NSS) testing. The coatings were observed to be conformal and uniform over rough surfaces, and contained some carbon and hydrogen as impurities. The electrochemical results showed that the Al(2)O(3) coating had superior sealing properties compared to the Ta(2)O(5) coating, and nanolaminates had properties in between those of Al(2)O(3) and Ta(2)O(5). However, in the NSS test the laminate-coated samples survived the best demonstrating long-term durability. Analysis of the laminate structure showed that for 40 and 80 nm laminates the best protection was achieved with 10 and 20 nm layers, respectively. (C) 2011 The Electrochemical Society. [DOI: 10.1149/2.061111jes] All rights reserved.