The combination of carbon nanotubes (CNTs) with polymers has been widely sought for the development of composite materials having high strength, high toughness, and in some cases multifunctional performance. Individual CNTs exhibit outstanding mechanical, electrical and thermal properties, and their nanometer-scale diameter combined with high aspect ratio give rise to a wide range of load transfer mechanisms with the organic materials, based on van der Waals or π interactions, or covalent bonding. While most early research on CNT-polymer composites focused on using CNTs as a filler or additive to polymer matrices at low loadings, recent emphasis has been placed on processing methods that combine organized CNT assembles, such as forests, sheets, or fibers, with polymers. In this emerging approach, a polymer is infiltrated into the already formed CNT network, leading to a final composite after additional processing. However, this method often results in heterogeneous polymer distribution and CNT aggregation which decrease drastically the mechanical properties of the composite. Herein, we propose to develop a new infiltration/in-situ polymerization composite manufacturing method which shows great potential to result in homogeneous composite morphology. We will use this method to evaluate the influence of the polymer structure on the mechanical properties of the final CNT-polymer composite system, as well as to study how a high CNT content may influence the polymerization kinetics.