A method of fabricating pillared graphene assembles alternate layers of graphene sheets and fullerenes to form a stable protostructure. Energy is added to the protostructure to break the carbon-carbon bonds at the fullerene-to-graphene attachment points of the protostructure and allow the bonds to reorganize and reform into a stable lower energy unitary pillared graphene nanostructure in which open nanotubes are conjoined between graphene sheets. The attachment points may be functionalized using tether molecules to aid in attachment, and add chemical energy to the system. The arrangement and attachment spacing of the fullerenes may be determined using spacer molecules or an electric potential.