A nano-scaled coating of titanium oxide (TiO2) on graphene (G) has been achieved via a novel atomic layer deposition (ALD) method. As a potential supercapacitor material, the TiO2-G composites exhibited a capacity of 75 F/g and 84 F/g at a scan rate of 10 mV/s for composites grown using 50 and 100 ALD cycles, respectively. The nearly identical Nyquist plots of the TiO2-G composites compared with those of pure graphene demonstrated that the composites possess excellent conductivity for charge transfer and open structures for ion diffusion. In addition, even with 3-4 times additional mass loading (maximum 3.22 mg/cm(2)), the composites exhibit no obvious degradation with respect to the electrochemical performance. This ALD approach presents a promising route to synthesize advanced graphene-based nanocomposites for supercapacitor applications. (C) 2012 The Electrochemical Society. [DOI: 10.1149/2.025204jes] All rights reserved.