Metal Organic Framework‐MXene Nanoarchitecture for Fast Responsive and Ultra‐Stable Electro‐Ionic Artificial Muscles

Abstract Electro‐ionic soft actuators, capable of continuous deformations replacing non‐compliant rigid mechanical components, attract increasing interest in the field of next‐generation metaverse interfaces and soft robotics. Here, a novel MXene (Ti₃C₂T_x) electrode anchoring manganese‐based 1,3,5‐benzenetricarboxylate metal‐organic framework (MnBTC) for ultrastable electro‐ionic artificial muscles is reported. By a facile supramolecular self‐assembly, the Ti₃C₂T_x‐MnBTC hybrid nanoarchitecture forms coordinate bond, hydrogen bond, and hydrophilic interaction with the conducting polymer of poly(3,4‐ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS), resulting in a mechanically flexible and electro‐ionically active electrode. The superior electrical and electrochemical performances of the electrode stem from the synergistic effects between intrinsically hierarchical nanoarchitecture of MnBTC and rapid electron transport behavior of Mxene, leading to fast diffusion and accommodation of ions in the ion‐exchangeable membrane. The developed artificial muscle based on Ti₃C₂T_x‐MnBTC is found to exhibit high bending displacement (12.5 mm) and ultrafast response time (0.77 s) under a low driving voltage (0.5 V), along with wide frequency response (0.1–10 Hz) and exceptional stability (98% retention at 43,200 s) without any distortion of actuation performance. Furthermore, the designed electro‐active artificial muscle is successfully used to demonstrate mimicry of eye motions including eyelid blinking and eyeball movement in a doll.