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A three dimensional (3D) polyaniline (PANI)–graphene nanoribbon (GNR)–carbon nanotube (CNT) composite, PANI–GNR–CNT, has been prepared via in situ polymerization of an aniline monomer on the surface of a GNR–CNT hybrid. Here, the 3D GNR–CNT hybrid has been conveniently prepared by partially unzipping the pristine multi-walled CNTs, while the residual CNTs act as “bridges” connecting different GNRs. The morphology and structure of the resulting hybrid materials have been characterized using transmission electron microscopy (TEM), scanning electron microscopy (SEM), Raman spectroscopy and X-ray diffraction (XRD). Electrochemical tests reveal that the hierarchical PANI–GNR–CNT composite based on the two-electrode cell possesses much higher specific capacitance (890 F g−1) than the GNR–CNT hybrid (195 F g−1) and neat PANI (283 F g−1) at a discharge current density of 0.5 A g−1 …