Ion-conducting polymers (ionomers) are an integral part of renewable energy-driven technologies. Proton exchange membrane fuel cells (PEMFCs) have already been incorporated into low-duty vehicles and are now being adopted in heavy-duty vehicles. Therefore, we need more durable and efficient fuel cell materials than ever. A major technical challenge of PEMFCs is the ion transport limitation at the ionomer-catalyst interface which negatively impacts the efficiency of the cells. The current state-of-the-art fuel cell ionomers (both fluorocarbon- and hydrocarbon-based) conduct protons efficiently in bulk, several tens of micron thick, free-standing membranes, but poorly in sub-micron thick films. This needs attention as sub-micron thick ionomer layers are used as catalyst binders on electrodes of PEMFCs and other energy conversion and storage devices. However, the nanoscale behavior of these existing ionomers within complex hydration environment is not well-understood yet. More importantly, ionomers are rarely designed to improve the thin film ion conduction properties. To address and overcome these issues, we do not only design innovative nanoscale materials characterization techniques to explore the distribution of ion conduction environment across ionomer films/membrane, but also design novel classes of ionomers inspired by natural living systems to facilitate ion conduction in thin films. We experimentally measure the ion conductivity, morphology, and mechanical properties, and combine them with computational studies to elevate our understanding of ion conduction mechanism within 10-200 nm thick films of these newly designed ionomers. The results suggest the great promise of these new classes of ionomers as efficiently ion-transporting catalyst binders for fuel cells, electrolyzers, and batteries.