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We report the growth of vertically aligned high-crystallinity silicon nanotube (SiNT) arrays on silicon substrate by means of a Ni–Au bilayer catalyst engineering technique. Nanotubes were synthesized through solid–liquid–solid method as well as vapor–liquid–solid. A precise evaluation utilizing atomic force microscopy and lateral force microscopy describes that the gold profile in Ni regions leads to the construction of multiwall SiNTs. The agreement of the structural geometry and stiffness of the obtained SiNTs with previous theoretical predictions suggest sp hybridization as the mechanism of tube formation. Apart from scanning electron and transmission electron microscopy techniques, photoluminescence spectroscopy (PL) has been conducted to investigate the formation of nanostructures. PL spectroscopy confirms the evolution of ultrafine walls of the silicon nanotubes, responsible for the observed …