Polypyrrole/carbon nanotube nanoscale composites were successfully fabricated by electrochemical deposition of polypyrrole over each of the carbon nanotubes in well-aligned large arrays. The thickness of the polypyrrole coating can be easily controlled by the value of the film-formation charge. For both thin (low film-formation charge) and thick (high film-formation charge) films, the polypyrrole coating on the surface of each nanotube is very uniform throughout the entire length, as observed by transmission electron microscopy.