Ionic electroactive polymer (IEAP) actuators are a class of electroactive polymer devices that exhibit electromechanical coupling through ion transport in the device. They consist of an ionomeric membrane coated with conductive network composites (CNCs) and conductive electrodes on both sides. A series of experiments on IEAP actuators with various types of CNCs has demonstrated the existence of a direct correlation between the performance of actuators and physical and structural properties of the CNCs. Nanostructure of CNC is especially important in hosting electrolyte and boosting ion mobility. This dissertation presents a series of systematic experiments and studies on IEAP actuators with two primary focuses: 1) CNC nanostructure, and 2) ionic interactions. A novel approach for fabrication of CNC thin-films enabled us to control physical and structural properties of the CNC thin-films. We, for the first time, facilitated use of layer-by-layer ionic self-assembly technique in fabrication of porous and conductive CNCs based on polymer and metal nanoparticles. Results were porous-conductive CNCs. We have studied the performance dependence of IEAP actuators on nano-composition and structure of CNCs by systematically varying the thickness, nanoparticle size and nanoparticle concentration of CNCs. We have also studied influence of the waveform frequency, free-ions and counterions of the ionomeric membrane on the performance and behavior of IEAP actuators. Using the LbL technique, we systematically changed the thickness of CNC layers consisting of gold nanoparticles (AuNPs) and poly(allylamine hydrochloride). It was observed that actuators consisting of thicker CNCs exhibit larger actuation curvature, which is evidently due to uptake of larger volume of electrolyte. Actuation response-time exhibited a direct correlation to the sheet-resistance of CNC, which was controlled by varying the AuNP concentration. It was observed that size and type of free-ions and counterion of ionomeric membrane are also influential on the actuation behavior or IEAP actuators and that the counterion of ionomeric membrane participates in the actuation process. / Ph. D.