Vertically-aligned carbon nanotubes possess many advantages for a wide range of multifunctional applications. Along with the controlled growth of aligned/micropatterned carbon nanotubes, surface modification of vertically-aligned carbon nanotubes are essential in order to meet specific requirements demanded for particular applications. While many innovative synthetic methods have been developed for controlled growth of vertically-aligned multiwalled and single-walled carbon nanotubes, various interesting physical and chemical approaches have recently been devised for functionalization of the constituent carbon nanotubes in vertically-aligned carbon nanotube arrays with their alignment being largely retained. In this article, recent developments in the controlled growth and modification of vertically-aligned carbon nanotubes for multifunctional applications are reviewed.