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Recently, two-dimensional graphene and its derivatives have received enormous interest for use in next-generation actuators due to their extraordinary electro-chemo-mechanical properties and facile preparation and functionalization. In particular, strong emphasis has been put on investigating high-performance ionic polymer actuators based on graphene materials to overcome problems such as low actuation performance, low durability, and high cost of fabrication. Nevertheless, the above issues still need to be resolved, and thus more advanced actuating materials have to be newly developed. Here, we address more recently developed graphene-based ionic polymer actuators, including promising graphene-based electrodes and graphene-reinforced nanocomposites, and highlight their remarkable material properties and high actuation performance, along with the significant roles of graphene. Specifically, the highly durable ionic polymer actuators are developed by employing crack-free and hydrophobic graphene papers as highly conductive, large-scale, flexible, and liquid impermeable electrodes. Moreover, we investigate high-performing graphene-reinforced nanocomposites, such as graphene–Nafion nanocomposites and graphene oxide–chitosan bio-nanocomposites, as promising ionic polymer membranes that possess significantly enhanced ion transport properties and electro-mechanical performance due to minute loading of functionalized graphene derivatives. These efforts will greatly contribute to high-performance ionic polymer actuators for practical applications in sensor/actuator integrated systems, biomimetic robots, active biomedical devices, human-friendly applications, soft haptic feedback systems, and next-generation soft electronics.

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