We demonstrate a technique for creating unique forms of pure sp(2)-bonded carbon and unprecedented heteromolecules. These new structures, which we refer to as sculpturenes, are formed by sculpting selected shapes from bilayer graphene, heterobilayers, or multilayered materials and allowing the shapes to spontaneously reconstruct. The simplest sculpturene is topologically equivalent to a torus, with dimensions comparable to those of fullerenes. The topology of these new molecular structures is stable against atomic-scale defects. We demonstrate that sculpturenes can form the basic building blocks of hollow, multiconnected structures, with potential applications to nanofluidics and nanoelectronics.