  The folding of paper, hide, and woven fabric has been used for millennia to
achieve enhanced articulation, curvature, and visual appeal for intrinsically
flat, two-dimensional materials. For graphene, an ideal two-dimensional
material, folding may transform it to complex shapes with new and distinct
properties. Here, we present experimental results that folded structures in
graphene, termed grafold, exist, and their formations can be controlled by
introducing anisotropic surface curvature during graphene synthesis or transfer
processes. Using pseudopotential-density functional theory calculations, we
also show that double folding modifies the electronic band structure of
graphene. Furthermore, we demonstrate the intercalation of C60 into the
grafolds. Intercalation or functionalization of the chemically reactive folds
further expands grafold's mechanical, chemical, optical, and electronic
diversity.
