The stringent requirements for a solid polymer electrolyte (SPE) in solid state devices such as batteries or supercapacitors are even more demanding when used in electromechanical actuators. Not only is the SPE expected to exhibit good conductivity, mechanical properties, adhesion and mechanical/electrical stability, but it must also be flexible, maintained good adhesion while flexing, be easily processible and be able to function in air. In this work polyacrylonitrile and Kynar based non-aqueous SPEs and water based polyacrylamide hydrogel ion source/sinks containing various perchlorate salts were tested for their applicability to polypyrrole and carbon nanotube actuators and supercapacitors. The results indicate that the optimum SPE for both polypyrrole and carbon nanotube actuators would be a polyacrylonitrile plasticized with propylene carbonate and ethylene carbonate containing 1.0M NaClO4. It is also apparent that the same SPE would be the most suitable for supercapacitor applications with these materials.