Carbon nanotubes and nanowires are important materials for new nanotechnology devices and sensors. Future opotoelectronic devices can be made from assemblies of nanostructured materials. One difficulty in preparing these assemblies from nanotubes is the lack of site-specific points of contact and the subsequent compliance of the linkage between nanoparticles. Using molecular mechanics and ab initio quantum mechanical calculations, we have modeled the assembly process of two and three-dimensional structures of carbon nanotubes. The linkers between the nanotubes consist of novel metalodendrimers. These dendrimers have multiple binding sites with chemically specified chirality. Most importantly, they are mechanically rigid. This enables the multidimensional constraints and geometry required for advanced electronic and optoelectronic devices. These computational results and the implied 3D nanostructures that are derived will be presented.