This work represents the properties of electrically aligned carbon nanotubes (CNT)/polycarbonate (PC) nanocomposites towards the development of hydrogen gas separation membranes. A fraction (0.1 weight %) of CNTs synthesized by chemical vapour deposition method have been dispersed homogeneously throughout PC matrix by ultrasonication. The alignment of CNT in PC matrix has been accomplished by applying an external electric field of 1250V/cm during solution casting. These nanocomposites have been studied by gas permeation, electrical, and dielectric constant measurements. Gas permeability measurements obtained here that electrically aligned nanocomposite membranes can be used as good hydrogen separating media. I-V characteristics and dielectric constant shows the enhancement in conductivity and permittivity of these nanocomposites. Overall experimental results exhibit here that alignment of CNTs in polymer matrix shows the dramatic improvement in mass and charge transport properties. Copyright (c) 2016 John Wiley & Sons, Ltd.