Graphene was oxidized with H2O2 to introduce additional anchoring sites for effective alumina coating on graphene by the sol-gel method. The X-ray photoelectron spectroscopy studies showed that the oxygen-containing groups such as hydroxyl group useful for coating were introduced by the oxidation. The transmission electron microscopy images and thermogravimetric analysis data demonstrated that the additional anchoring sites enhanced the efficiency of the alumina coating. A small amount of alumina-coated graphene synergistically improved the thermal conductivity of the alumina sphere/thermoplastic polyurethane (TPU) composite without any increase in the electrical conductivity, because the electrical conductivity of graphene effectively decreased by the alumina coating. Moreover, the synergistic effect of a small amount of graphene was enhanced by the alumina coating, and the stiffening of the alumina sphere/TPU composite due to the added graphene was alleviated by the alumina coating. (C) 2015 Elsevier B.V. All rights reserved.