A natural clay halloysite, which is a kind of aluminosilicate with a predominantly nanosized hollow tubular structure, was modified by polymers achieving polymer-halloysite composite nanotubes. Polymer chains can grow from both interior and exterior surfaces of the halloysite nanotubes by atom transfer radial polymerization (ATRP). Eventually, the composite nanotubes were evolved to a core-shell coaxial structure after the interior cavity was fully covered by the polymer. After dissolution of the halloysite template, polymeric nanotubes and nanowires were derived. The composition could be controlled from polymer to carbon after being treated at high temperature. The idea can be extended to a cast halloysite fabric resulting nonwoven composites, which had some interesting wettability.