With the rapid development of autonomous and intelligent devices driven by soft actuators, ion soft actuators in flexible intelligent devices have several advantages over other actuators, including their light weight, low voltage drive, large strain, good flexibility, fast response, etc. Traditional ionic polymer metal composites have received a lot of attention over the past decades, but they suffer from poor driving performance and short service lives since the precious metal electrodes are not only expensive, heavy, and labor‐intensive, but also prone to cracking with repeated actuation. As excellent candidates for the electrode materials of ionic soft actuators, carbon‐based nanomaterials have received a lot of interest because of their plentiful reserves, low cost, and excellent mechanical, electrical, and electrochemical properties. This research reviewed carbon‐based nanomaterial electrodes of ion soft actuators for flexible smart devices from a fresh perspective from 1D to 3D combinations. The design of the electrode structure is introduced after the driving mechanism of ionic soft actuators. The details of ionic soft actuator electrodes made of carbon‐based nanomaterials are then provided. Additionally, a summary of applications for flexible intelligent devices is provided. Finally, suggestions for challenges and prospects are made to offer direction and inspiration for further development.