The materials used in many branches of engineering for actuation applications are typically heavy, nonflexible and require high driving power, so their practicality for creating biomimetic systems is limited. Due to their unique combination of electrical and mechanical properties, carbon nanotubes have attracted a great deal of interest for use as electromechanical actuators. Individual carbon nanotubes combine excellent electrical and thermal conductivities with remarkable mechanical properties. They are also currently considered the strongest and stiffest materials known. However, these properties have yet to be effectively transferred when the nanotubes are attempted to be assembled into useful macroscopic forms. A practical approach to manufacture manageable structures of carbon nanotubes for engineering applications is to assemble them into buckypapers. Buckypapers are sheets of highly entangled single- or multiwalled nanotubes held together by entanglement and van der Waals interactions. These structures provide sufficient mechanical and good electrochemical properties to study their actuator performance and applications. To incorporate buckypaper actuators into engineering systems, it is of high importance to understand their material property-actuation performance relationships in order to model and predict the behavior of these actuators. The electromechanical actuation of macroscopic buckypaper structures and their actuators, including single and multi-walled carbon nanotube buckypapers and aligned single-walled nanotube buckypapers, were analyzed and compared. From the experimental evidence, this paper discusses the effects of the fundamental material properties, including Young modulus and electrical double layer properties, on actuation performance of the resultant actuators.