Homogeneously distributed self-assembling hybrid graphene-based aerogels with 3D interconnected pores, employing three types of carbohydrates (glucose, beta-cyclodextrin, and chitosan), have been fabricated by a simple hydrothermal route. Using three types of carbohydrates as morphology oriented agents and reductants can effectively tailor the microstructures, physical properties, and electrochemical performances of the products. The effects of different carbohydrates on graphene oxide reduction to form graphene-based aerogels with different microcosmic morphologies and physical properties were also systemically discussed. The electrochemical behaviors of all graphene-based aerogel samples showed remarkably strong and stable performances, which indicated that all the 3D interpenetrating microstructure graphene-based aerogel samples with well-developed porous nanostructures and interconnected conductive networks could provide fast ionic channels for electrochemical energy storage. These results demonstrate that this strategy would offer an easy and effective way to fabricate graphene-based materials. (c) 2013 Elsevier Inc. All rights reserved.