Throughout the evolution of human technologies, electronic-based actuators have been unreplaceable. These actuators can provide superior power and speed in comparison to biological tissue. However, complexity and bulkiness are two of the major weaknesses that prevent electronic-based actuators from being implemented in biomimicking and biomedical applications. Recent advances in material sciences have suggested the possibility of flexible material-based actuators. These “smart material” actuators can be constructed by combining different composite materials, and motion or deformation can be observed once the actuator is subjected to a proper stimulus. This thesis presents a series of studies that focus on the development of novel active hybrid composites. Starting with a well-known polymeric blend shape memory polymer (SMP) and electrothermal actuator (ETA) system, the composites were first modified with nanoparticles to achieve room temperature deformability. The plasticizing effect was then utilized to enhance the actuation temperature, while conductive filler was implemented to enable electroactive ability. Lastly, a novel 4D printing fabrication process was presented, which demonstrated the possibility of using the material-based actuators in artificial muscles and soft robotic applications.