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State of the art smart materials such as piezo ceramics or electroactive polymers cannot feature both, mechanical stiffness and high active strain. Moreover, properties like low density, high mechanical stiffness and high strain at the same time driven by low energy play an increasingly important role for their future application. Carbon nanotubes (CNT), show this behavior. Their active behavior was observed 1999 the first time using paper-like mats made of CNT. Therefore the CNT-papers are electrical charged within an electrolyte thus forming a double- layer. The measured deflection of CNT material is based on the interaction between the charged high surface area formed by carbon nanotubes and ions provided by the electrolyte. Although CNT-papers have been extensively analyzed as well at the macro-scale as nano-scale there is still no generally accepted theory for the actuation mechanism. This paper focuses on investigations of the actuation mechanisms of CNT-papers in comparison to vertically aligned CNT-arrays. One reason of divergent results found in literature might be attributed to different types of CNT samples. While CNT-papers represent architectures of short CNTs which need to bridge each other to form the dimensions of the sample, the continuous CNTs of the array feature a length of almost 3 mm, along which the experiments are carried out. Both sample types are tested within an actuated tensile test set-up under different conditions. While the CNT-papers are tested in water-based electrolytes with comparably small redox-windows the hydrophobic CNT-arrays are tested in ionic liquids with comparatively larger redox-ranges. Furthermore an in-situ micro tensile test within an SEM is carried out to prove the optimized orientation of the MWCNTs as result of external load. It was found that the performance of CNT-papers strongly depends on the test conditions. However, the CNT-arrays are almost unaffected by the conditions showing active response at negative and positive voltages. A micro alignment as result of tensile stress can be proven. A comparison of both results point out that the actuation mechanism strongly depends on the weakest bonds of the architectures: Van-der-Waals-bonds vs. covalent C-bonds.
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