The present invention generally relates to nanotechnology and, in particular, to wireframe nanostructures which may be formed from nucleic acids. In various aspects, the invention relates to molecular structures having a plurality of vertices and pathways connecting the vertices, which may be formed from nucleic acids, including bundles or tubes of nucleic acids. Such molecular structures may form shapes such as icosahedrons, octahedrons, tetrahedrons, or other polyhedra, which may define an interior space. The interior space may be used, for example, to contain a molecule for further study, or to contain a molecule for drug delivery purposes. In some cases, the molecular structure may be stabilized using relatively short nucleic acid strands that interact with two or more nucleic acid portions within the structure, thereby substantially immobilizing the portions relative to each other. Other aspects of the invention relate to techniques for forming such molecular structures, techniques for using such molecular structures, techniques of promoting such molecular structures, kits involving such molecular structures, and the like.