In some embodiments, the present invention is directed to methods of fully integrating CNTs and the surrounding polymer matrix in CNT/polymer composites. In some such embodiments, such integration comprises interfacial covalent bonding between the CNTs and the polymer matrix. In some such embodiments, such interfacial covalent bonding is provided by a free radical reaction initiated during processing. In some such embodiments, such free radical initiation can be provided by benzoyl peroxide. In some or other embodiments, the present invention is directed to CNT/polymer composite systems, wherein the CNTs within such systems are covalently integrated with the polymer. In some or other embodiments, the present invention is directed to articles of manufacture made from such CNT/polymer composite systems.