Bucky gel actuator (BGA) is a type of electro‐active polymer that bends when stimulated by an electric field. Its operation is affected by a matrix network, which has two opposite effects on ion migration and material strength properties of the actuator. Therefore, designing a BGA with more deflection or more strength demands the study of matrix structural properties. In this paper, polyvinylidene fluoride (PVDF) was used as the polymer matrix in BGA composites, and the degree of crystallinity and the fraction of
β phase were calculated using X‐ray diffraction and Fourier Transform Infrared spectroscopy respectively to investigate the matrix structural properties. Furthermore, Raman spectroscopy analysis was utilized for phase characterization. Several composite films with various components including electrode and electrolyte layers of BGA were prepared by the drop‐casting method in two different conditions to study the effects of PVDF concentration in dimethylacetamide solvent, drying temperature, and additive materials on the matrix structural properties for the first time. It was observed that low concentrations of PVDF in dimethylacetamide solvent coupled with a high drying temperature in a carbon nanotube‐based BGA in contrast with using a graphene‐based BGA, had the lowest degree of crystallinity and
β phase fraction. POLYM. COMPOS., 39:E1208–E1215, 2018. © 2018 Society of Plastics Engineers