In recent decades, micro and nanoscale technologies have become cutting-edge frontiers in material science and device developments. This worldwide trend has induced further improvements in actuator production with enhanced performance. A main role has been played by nanostructured carbon-based materials, i.e., carbon nanotubes and graphene, due to their intrinsic properties and easy functionalization. Moreover, the nanoscale decoration of these materials has led to the design of doped and decorated carbon-based devices effectively used as actuators incorporating metals and metal-based structures. This review provides an overview and discussion of the overall process for producing AC actuators using nanostructured, doped, and decorated carbon materials. It highlights the differences and common aspects that make carbon materials one of the most promising resources in the field of actuators.