In recent years, carbon nanotubes (CNTs) based artificial muscles attract many research attentions due to their superior actuation forces and high work density. Previous research successfully demonstrated that bundles of CNTs joined by Van der Waal’s forces can behave as actuators when submersed in electrolyte with external voltage applied to the CNTs. Such behavior can be explained by the rearrangement of atomic structure of the CNTs and Coulombic forces; which were both induced by ions exchange between the CNT bundles and the electrolyte. It was suggested that the performance of CNT based actuators can be further improved by enhancing the interfacial surface areas via fiber alignment. Currently, most of the CNT based actuators are fabricated via direct drawing of the “CNT forests”. Although commonly practiced in laboratory, the growth of ‘CNT forests’ still requires expensive and challenging techniques such as chemical vapor deposition (CVD). In this study, we present the results of CNT/polymer composites actuator fabricated by electrospinning processes. Such methods utilized electrospinning for manipulating the alignment and connection between individual CNTs. Compared to the results of different fabrication techniques shown in the literature, similar actuation behavior is found and reported in this study.