Metrics & MoreArticle Recommendations CONSPECTUS: Ionic polymer−metal composites (IPMCs) are one kind of artificial muscles that can realize energy conversions in response to external stimulus with merits of lightweight, scalability, quick response, and flexibility and have been treated as an important platform in artificial intelligence, such as bionic robotics, smart sensors, and micro-electromechanical systems. It is wellknown that IPMC devices are mainly composed of one electrolyte layer laminated with symmetric electrode layers and realize energy conversion based on ion migration and redistribution inside the devices. However, several critical issues have greatly impeded the practical applications of IPMC devices, including metal electrode cracks, metal−polymer interface detachment, and water loss in the electrolyte. In the past decade, our group and collaborators have made attempts to address the mentioned critical issues with the purpose of accelerating practical applications of IPMC devices. First, in order to address the metal electrode cracks, we have developed various electrode materials to replace the metal electrode material, such as black phosphorus and graphdiyne. These materials display superior electrical and mechanical properties with enhanced material stability without cracking. Second, to address metal−polymer interface detachment, we have designed robust interfaces for IMPC devices with vertical array structures. The asprepared interfaces present high ionic conductivity with excellent mechanical stability under bending states. As a result, the IPMC devices deliver high working stability exceeding a million cycles under air conditions. Third, in order to avoid water loss in the electrolyte, especially at ambient conditions, we have developed ionogel electrolytes containing highly stable ionic liquids as active ion sources. The ionogel electrolytes effectively prevent water loss in conventional water-containing electrolytes, just like Nafion electrolytes and greatly improve the working stability of IPMC devices. After addressing the key issues of IPMC devices, we finally obtained many high-performing IPMC devices and explored various intelligent applications of them. For instance, we have demonstrated the smart functions of IPMC devices as sensitive strain sensors, such as sign language recognition, handwriting detection, and human muscle monitoring. In addition, we have developed bionic flying robots with a vibration frequency as high as 30 Hz with the aid of high-performance IPMC actuators. A medical catheter based on IPMC actuators has been put forward by our group and can realize multiple degrees of freedom deformation under a low driving voltage of 2.5 V, which presents great potential for application in medical instruments. Lastly, a perspective on critical challenges and future research directions on IPMC materials and devices is highlighted for accelerating practical application.