This dissertation, including an introductory chapter, four main chapters detailing each study, and a concluding chapter, presented four interdisciplinary studies focused on developing bioinspired nanomaterials with novel combinations of properties for use in ionic artificial muscles. Beyond nanomaterials and ionic artificial muscles, the research spanned polymer synthesis, micelle science, nanocomposite, CTF synthesis, electrochemistry, bioinspiration and biomimetics, design mechanics, and soft robotics.