Nanostructures are linked to many areas of science and technology. A cornerstone of our current research is the practical development of boron cluster-based, nanostructured materials-by-design. It is now possible to imagine and predictably model properties, synthesis procedures, manufacturing processes, and to functionally integrate engineering principles. Super-properties such as hardness, wear, resistance, superconductivity, energy storage, boron neutron capture therapy, will benefit from the strategic application of boron Nanostructures. We have determined and predicted a number of structures via theoretical models as quasi-planar clusters and sheets, hollow spheres, and nanotubes, based on Ab Initio first-principles methods. Some have been confirmed experimentally.