Lithographically defined microporous templates in conjunction with the atomic layer deposition (ALD) technique enable remarkable control of complex novel nested nanotube structures. So far three-dimensional control of physical process parameters has not been fully realized with high precision resolution, and requires optimization in order to achieve a wider range of potential applications. Furthermore, the combination of composite insulating oxide layers alternating with semiconducting layers and metals can provide various types of novel applications and eventually provide unique and advanced levels of multifunctional nanoscale devices. Semiconducting TiO₂ nanotubes have potential applications in photovoltaic devices. The combination of nanostructured semiconducting materials with nested metal nanotubes has the potential to produce novel multifunctional vertically-ordered three-dimensional nanodevices. Platinum growth by ALD has been explored, covering the initial stages of the thin film nucleation process and the synthesis of high aspect ratio nanotube structures. The penetration depth of the Pt into porous templates having various pore sizes and aspect ratios has been investigated. Several multi-walled nested TiO₂–Pt nanotubes in series have been successfully fabricated using microporous Si templates. These innovative nested nanostructures have the potential to produce novel multifunctional vertically-ordered three-dimensional nanodevices in photovoltaic and sensing technologies.