A method of forming aerogels includes mixing a plurality of polymers or aromatic molecules, a solvent, and a plurality of carbon nanotubes (CNTs) or graphene including structures to form a mixture, where the polymers or aromatic molecules have at least one crosslinkable structure. A solid gel is formed including a plurality of supramolecular structures from the mixture. The plurality of supramolecular structures include a plurality of the polymers or aromatic molecules secured by π-π bonds to the outer surface of the CNTs or graphene including structures. The solid gel includes a portion of the solvent trapped therein. The plurality of supramolecular structures are crosslinked and then dried to remove the solvent trapped therein to form the aerogel.