Recently, considerable achievements have been made with the advancements of smart structures, which are known for their controlled deformation, self-repair, and sensing characteristics. Such capabilities have significant potential in the field of bionics. 3D printing methods have revolutionized the high-resolution integrated manufacturing of complex smart structures, resulting in new types of soft robots, actuators, wearable flexible electronics, and biomedical equipment. There is therefore a need for academia and industry to receive an update on the status of these tools. For this reason, herein, a comprehensive overview of the latest progress in printing methods, materials, and applications of various smart structures is provided. Temperature-and electromagnetic-responsive smart structures are highlighted, in addition to self-healing and smart-sensing devices. Current exigencies and future development trends of 3D printing methods and smart structures are also summarized.