Carbon nanomaterials show great promise for a wide range of applications due to their excellent physicochemical and electrical properties. Since their discovery, the state-of-the-art has expanded the scope of their application from scientific curiosity to impactful solutions. Due to their tunability, carbon nanomaterials can be processed into a wide range of formulations and significant scope exists to couple carbon structures to electronic and electrochemical applications. In this paper, the electrochemical performance of various types of CNT films, which differ by the number of walls, diameter, chirality and surface chemistry is presented. We show that by controlling the CNT structure we can manufacture macroscopic devices precisely tailored for a wide range of applications, with the focus on energy storage devices and super-capacitors.