Graphene/NiAl layered double-hydroxide (LDH) composite with high capacitive properties has been prepared in a friendly one-step process. It is found that NiAl-LDH is formed in the addition of precipitator agent (NaOH and NaNO3) by hydrothermal method, at the same time graphene oxide (GO) is reduced to graphene. The morphology and structure of the obtained material are examined by X-ray diffraction (XRD), Brunauer-Emmett-Teller (BET), transmission electron microscope (TEM), and scanning electron microscope (SEM) techniques. It is revealed that the NiAl-LDH disperses well on the surface of graphene and the formation of NiAl-LDH nanoparticles is beneficial to the peeling of graphene (RGO). More importantly, the addition of NiAl-LDH to graphene endows the materials with desirable specific surface areas and higher porosity. These structural advantages result in higher specific capacitance compared with pristine graphene. Electrochemical property investigations show that the graphene/NiAl-LDH had a higher specific capacitance than graphene. Crown Copyright (C) 2013 Published by Elsevier Inc. All rights reserved.