Cobalt MOF‐Based Porous Carbonaceous Spheres for Multimodal Soft Actuator Exhibiting Intricate Biomimetic Motions

The advancement of active electrode materials is essential to meet the demand for multifaceted soft robotic interactions. In this study, a new type of porous carbonaceous sphere (PCS) for a multimodal soft actuator capable of both magnetoactive and electro‐ionic responses is reported. The PCS, derived from the simultaneous oxidative and reductive breakdown of specially designed cobalt‐based metal–organic frameworks (Co‐MOFs) with varying metal‐to‐ligand ratios, exhibits a high specific surface area of 529 m2 g−1 and a saturated magnetization of 142.7 Am2 kg−1. The size of the PCS can be controlled through the Ostwald ripening mechanism, while the porous structure can be regulated by adjusting the metal‐to‐ligand mol ratio. Its exceptional compatibility with poly(3,4‐ethylene‐dioxythiophene)‐poly(styrenesulfonate) enables the creation of uniform electrode, crucial for producing soft actuators that work in both magnetic and electrical fields. Operated at an ultralow voltage of 1 V, the PCS‐based actuator generates a blocking force of 47.5 mN and exhibits significant bending deflection even at an oscillation frequency of 10 Hz. Employing this simultaneous multimodal actuation ensures the dynamic and complex motions of a balancing bird robot and a dynamic eagle robot. This advancement marks a significant step toward the realization of more dynamic and versatile soft robotic systems. Porous carbonaceous sphere derived from cobalt metal–organic frameworks is suggested to develop multimodal electro‐ionic and magnetoactive soft actuators with expanded bandwidth and strong force actuation. These actuators are then utilized to demonstrate the high‐frequency motion of a balancing bird and a dynamic eagle robot having a magneto‐responsive claw.