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We have successfully coated CNTs with either positively or negatively charged polyelectrolytes employing Van der Waals interactions between nanotubes and polyelectrolyte molecules, without any previous chemical modification of the nanotubes walls. Polymer adsorption of polyelectrolytes was performed in an ethanolic solution, followed by redispersion in water. The surface coating was verified with ζ-potential measurements and SEM. A sequential assembly of polyelectrolyte layers on top of the polyelectrolyte modified nanotubes has been achieved from a water solution following the layer-by-layer technique. The assembly of polyelectrolytes from water on CNTs deposited on a surface has also been shown with QCM-D. Then, polyelectrolyte coated CNTs have been used as positive and negative blocks in the templating of layer-by-layer films.