This report highlights recent progress in the fabrication of vertically aligned carbon nanotubes (VA-CNTs) on silicon-based materials. Research into these nanostructured composite materials is spurred by the importance of silicon as a basis for most current devices and the disruptive properties of CNTs. Various CNT attachments methods of covalent and adsorptive nature are critically compared. Selected examples of device applications where the VA-CNT on silicon assemblies are showing particular promise are discussed. These applications include field emitters, filtration membranes, dry adhesives, sensors and scaffolds for biointerfaces.