A three-dimensional hierarchical graphene/polypyrrole aerogel (GPA) has been fabricated using graphene oxide (GO) and already synthesized one-dimensional hollow polypyrrole nanotubes (PNTs) as the feedstock. The amphiphilic GO is helpful in effectively promoting the dispersion of well-defined PNTs to result in a stable, homogeneous GO/PNT complex solution, while the PNTs not only provide a large accessible surface area for fast transport of hydrate ions but also act as spacers to prevent the restacking of graphene sheets. By a simple one-step reduction self-assembly process, hierarchically structured, low-density, highly compressible GPAs are easily obtained, which favorably combine the advantages of graphene and PNTs. The supercapacitor electrodes based on such materials exhibit excellent electrochemical performance, including a high specific capacitance up to 253 F g(-1), good rate performance, and outstanding cycle stability. Moreover, this method may be feasible to prepare other graphene-based hybrid aerogels with structure-controllable nanostructures in large scale, thereby holding enormous potential in many application fields.