One of the key bottlenecks of nanotechnology is the inability to translate the amazing properties of individual nanostructures (e.g. carbon nanotubes, nanoparticles etc.) to larger scales due to the inability to engineer them with control. We have been pursuing approaches to scalably produce three-dimensional nanostructured materials with control of the interfaces between these individual building blocks. Good control of this building process could yield unique nanostructured materials with tunable density, structure, morphology and properties and could lead to several interesting applications.