Bimetallic AuPt nanoparticles prepared by radiolysis with Au/Pt atomic ratios of 1.2 and 1.8 were deposited onto silica and calcined to remove the stabilizing polymers. During this sequence, they lose their core shell structure and restructure as alloys. FTIR and XPS provide evidence for further AuPt NP restructuring under CO exposure and CO oxidation with Pt surface enrichment. A promoting effect of Au is found on the CO oxidation kinetics in the AuPt catalyst with the lower Au/Pt ratio. This effect is attributed to an electron enrichment of the Pt surface atoms due to charge transfer from Au to Pt, as indicated by XPS and CO-FTIR. (C) 2011 Elsevier Inc. All rights reserved.