This study describes an atomic layer deposition (ALD) approach for the fabrication of Pt nanocatalysts supported on graphene oxide (GO) sheets and their electrocatalytic performance in electro-oxidation of formic acid. The ALD process for forming the Pt atomic layer involves two self-limiting reactions and, thus, induces the decoration of ALD-Pt on the edges of GO sheets with the presence of dangling bonds and oxygen functionalities. The resultant ALD-Pt catalyst on GO sheets offers better catalytic activity, CO tolerance, and long-term stability than those on commercial carbon support. On the basis of the results, the ALD approach described here can be applied to the design of novel catalytic materials for a variety of energy-storage applications, for example, high-performance fuel cells. Copyright (c) 2012, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.