Biocompatible electromechanical actuator devices are sought for numerous applications including implantable valves, drug delivery devices, surgical tools or dynamic artificial tissues. For this purpose, we have developed single component, metal-free actuators based on composites composed of the polypeptide silk fibroin (for mechanical strength, flexibility, biocompatibility) and poly(pyrrole) or poly(3,4-ethylenedioxythiophene) (stimuli-responsive conducting polymers). Chemical modification techniques were developed to produce free-standing films with bilayer or trilayer-type structures, with unmodified silk comprising the core of the film and an interpenetrating network (IPN) of silk and conducting polymers on the surface. The IPN structure prohibits delamination of the conducting polymer, resulting in a durable device structure. The fabrication of these composites is quite versatile, allowing the chemical composition, surface morphology, and device architecture to be varied independently. Here we will present the effects of these variables on the electrochemical stability, free-end bending actuation performance, strain and force generation of these composite films in a biologically-relevant environment.