Multilayer electroactive polymer actuators consisting of polypyrrole films electropolymerized on a passive polymer membrane core have been harnessed as a source of simple actuation. As an integral component of the actuator, the membrane plays a vital role in the transport of ionic species and largely dictates the stiffness of the layered configuration, yet in past studies the specification of the membrane has remained largely arbitrary. In this investigation, we use quasi-static and dynamic mechanical analysis to investigate the impact of the mechanical properties of the membrane on the actuation response of polypyrrole-based trilayer bending actuators. Candidate materials with distinctly varied microcellular morphologies are identified and include polyvinylidene difluoride, nylon, and nitrocellulose. The quasi-static stress-strain response and the frequency-dependent viscoelastic nature of the candidates are then evaluated. On the basis of mechanical properties these results indicate that polyvinylidene difluoride membranes are superior to the other candidates for application as trilayer actuator cores. Bis(trifluoromethane)sulfonimide doped polypyrrole actuators with polyvinylidene difluoride cores and nylon cores are then fabricated under various synthesis conditions and their electromechanical actuation behavior is reported.