Oxygen reduction reaction catalysts based on precious metals such as platinum or its alloys are routinely used in fuel cells because of their high activity. Carbon-supported materials containing metals such as iron or cobalt as well as nitrogen impurities have been proposed to increase scalability and reduce costs, but these alternatives usually suffer from low activity and/or gradual deactivation during use. Here, we show that few-walled carbon nanotubes, following outer wall exfoliation via oxidation and high-temperature reaction with ammonia, can act as an oxygen reduction reaction electrocatalyst in both acidic and alkaline solutions. Under a unique oxidation condition, the outer walls of the few-walled carbon nanotubes are partially unzipped, creating nanoscale sheets of graphene attached to the inner tubes.