FeOx-supported gold nanocatalyst is one of the most active catalysts for low-temperature CO oxidation. However, the origin of the high activity is still in debate. In this work, using a combination of surface-sensitive in situ FT-IR, Raman spectroscopy, and microcalorimetry, we provide unambiguous evidence that the surface lattice oxygen of the FeOx support participates directly in the low-temperature CO oxidation, and the reaction proceeds mainly through a redox mechanism. Both the presence of gold and the ferrihydrite nature of the FeOx support promote the redox activity greatly. Calcination treatment has a detrimental effect on the redox activity of the Au/FeOx, which in turn decreases greatly the activity for low-temperature CO oxidation. The gold-assisted redox mechanism was also extended to other metal-supported FeOx catalysts, demonstrating the key role of the FeOx support in catalyzing the CO oxidation reaction. (c) 2012 Elsevier Inc. All rights reserved.