In this study, we compared the wetting and electrowetting properties of a planar parylene (poly(p-xylylene)) film to those of a nanostructured parylene film. To generate the nanostructured film, we used an aligned array of multiwalled carbon nanotubes as a template; a thin coating of parylene was deposited on the nanotube template to generate a parylene film with a nanoscale roughness structure. Static contact angle measurements indicated a very significant increase in the water contact angle from similar to 73 degrees for planar parylene to similar to 110 degrees for the nanotemplated parylene. In addition, we performed electrowetting experiments to dynamically tune the contact angle by application of electric potential. Interestingly, the flat parylene film showed contact angle saturation at an applied voltage of similar to 40 V, while the nanotemplated parylene film did not experience saturation in the contact angle response even for voltages up to 80 V. These results show that engineering a nanoscale roughness structure to a polymer film results in significant changes to the wetting and electrowetting properties of the polymer.