Abstract Conventional Nafion-based ionic actuators suffer from hydration-dependent ion transport and a long-standing trade-off between ionic conductivity and mechanical stiffness, which limits force generation and stable high-frequency operation. Here, we report a PEG-silica-hybridized ionic electroactive Nafion (Ps-iEN) that introduces a mesoscale interfacial ion-transport network via PEG-mediated surface functionalization.