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The excellent optoelectronic, mechanical, and thermal properties of carbon nanotubes have made them very attractive for a wide range of potential applications. However, many applications require the growth of aligned carbon nanotubes with surface modification. We have developed a simple pyrolytic method for large-scale production of aligned carbon nanotube arrays perpendicular to the substrate. These aligned carbon nanotube arrays can be transferred onto various substrates of particular interest (e.g., polymer films for organic optoelectronic devices) in either a patterned or non-patterned fashion. The well-aligned structure further allows us to prepare aligned coaxial nanowires by electrochemically depositing a concentric layer of an appropriate conducting polymer onto the individual aligned carbon nanotubes. This approach is particularly attractive, as it allows surface characteristics of the aligned carbon nanotubes to be tuned to meet specific requirements for particular applications while their alignment structure can be largely retained. These aligned carbon nanotubes with tunable surface characteristics are of great significance to various practical applications. In this paper, we demonstrate the use of the conducting-polymer-coated aligned carbon nanotubes for electrochemical sensing applications. © 2003 American Vacuum Society.