The gas barrier properties and electrochemical redox behavior of aniline oligomer-derivated electroactive polyimide (EPI) hybrid with graphene oxide (GO) were investigated as a function of the content of amino-capped aniline trimer (ACAT) and GO. A series of EPI thin films were prepared from a non-coplanar dianhydride, [2, 2-bis [4- (dicarboxyphenoxy) phenyl] propane dianhydride] (IDPA), and two types of diamines, 4, 4'-diaminodiphenyl ether (ODA) and ACAT, in DMAc solvent. The effects of ACAT contents on the mechanical and barrier properties of EPI were investigated. In order to further reduce the water-vapor-transmission-rate (WVTR) and oxygen-transmission-rate (OTR) of EPI, silk-like GO nanosheets were incorporated with EPI. The high aspect ratio of GO successfully extends the diffusion pathway of the gas barrier in the EPI matrix and thus serves as an excellent barrier material for EPI. (9 refs)