Capacitive deionization (CDI) is a novel ion removal technology that uses static electrical force to drive ions to the charged electrode and stores the ions into porous structure of the electrode. Graphene and graphene nanocomposites are considered promising materials for electrodes because of its good conductivity and extraordinarily high specific surface area. Graphene/Polyaniline nanocomposite was chosen that aims to increase the ion-electrosorption capacitance of graphene. In this work, graphene nanosheets were obtained by reducing oxidized graphite flasks. Graphene/Polyaniline (G/PANI) nanocomposites were synthesized by chemical polymerization of aniline in the presence of dispersed graphene sheets. The morphology and electrochemical property of the composite were characterized. The ion removal performance of the composite was determined by using a membrane capacitive deionization (CDI) bench-scale system.