Polyaniline (PANi) is synthesized on a highly ordered and flexible graphene paper ( GNP) by in situ polymerization followed by folding the 2D composite paper into a 3D structure. The thermoelectric properties of this novel composite structure is improved as a result of the formation of an electrically connected, thermally disconnected structure due to the interconnected folds within the composite that allow electrons to conduct while discouraging phonon transport. Mechanical compaction on the folded sample is essential to produce a consolidated sample. ZT of this novel composite is an order of magnitude higher than that of neat GNP paper. (C) 2014 Elsevier B.V. All rights reserved.