ABSTRACTNanocomposites based on polycarbonate (PC) and different amounts of untreated graphene nanoplatelets (GnP) (from 1 to 7 wt %) were prepared by melt blending. The nanocomposites were thoroughly characterized employing the following techniques: broad band dielectric spectroscopy, thermally stimulated depolarization currents, differential scanning calorimetry, tensile testing, dynamic mechanical thermal analysis, and water vapor, carbon dioxide and oxygen permeability measurements. The presence of a MWS relaxation mode indicated the accumulation of electrical charges trapped at the interfaces of the polycarbonate with graphene 2D platelets. The addition of GnP produced nanocomposite materials with enhanced mechanical and barrier properties. The melt mixed PC/graphene nanocomposites prepared here exhibit well‐balanced properties, even though unmodified graphene nanoplatelets were used. In addition, the nanocomposites were obtained by a single extrusion process, which is easily scalable for industrial applications. © 2016 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017, 134, 44654.