Electroactive thin-film polymers are increasingly being used as sensors and actuators in aerospace structures [1,2]. They also have significant potential for applications in muscle mechanisms and micro-electro-mechanical systems (MEMS). In these applications, polymer films of thickness varying between 20 and 300 μm are utilized. Actuation of these polymers is attributed to piezoelectric, electrostrictive or electrostatic effects. Recent investigations suggest that polymers may produce striction which can be stronger than that delivered by electroactive ceramics. Such response may be produced by polymers with isotacticity or syndiotacticity in their molecular structure, where tacticity is the position of a pendant polymer group with a strong dipole moment that is mounted on a backbone polymeric chain.