Over the past few decades, carbon materials, including fullerenes, carbon nanotubes, graphene, and porous carbons, have achieved tremendous success in the fields of energy, environment, medicine, and beyond, through their development and application. Due to their unique physical and chemical characteristics for enabling simultaneous interaction with ions and transport of electrons, carbon materials have been attracting increasing attention in the emerging field of iontronics in recent years. In this review, we first summarize the recent progress and achievements of carbon-based iontronics (ionic sensors, ionic transistors, ionic diodes, ionic pumps, and ionic actuators) for multiple bioinspired applications ranging from information sensing, processing, and actuation, to simple and basic artificial intelligent reflex arc units for the construction of smart and autonomous iontronics. Additionally, the promising potential of carbon materials for smart iontronics is highlighted and prospects are provided in this review, which provide new insights for the further development of nanostructured carbon materials and carbon-based smart iontronics.