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Advances in the understanding of nanoscale ionic processes in solid‐state thin films have led to the rapid development of devices based on coupled ionic–electronic effects. For example, ion‐driven resistive‐switching (RS) devices have been extensively studied for future memory applications due to their excellent performance in terms of switching speed, endurance, retention, and scalability. Recent studies further suggest that RS devices are more than just resistors with tunable resistance; instead, they exhibit rich and complex internal ionic dynamics that equip them with native information‐processing capabilities, particularly in the temporal domain. RS effects induced by the migration of different types of ions, often driven by an electric field, are discussed. It is shown that, by taking advantage of the different state variables controlled by the ionic processes, important synaptic functions can be faithfully implemented in solid‐state devices and networks. Recent efforts on improving the controllability of ionic processes to optimize device performance are also discussed, along with new opportunities for material design and engineering enabled by the ability to control ionic processes at the atomic scale.

Rapid advances in the semiconductor industry, driven largely by device scaling, are now approaching fundamental physical limits and face severe power, performance, and cost constraints. Multifunctional materials and devices may lead to a paradigm shift toward new, intelligent, and efficient computing systems, and are being extensively studied. Herein examines how, by controlling the internal ion distribution in a solid‐state film, a material's chemical composition and physical properties can be reversibly reconfigured using an applied electric field, at room temperature and after device fabrication. Reconfigurability is observed in a wide range of materials, including commonly used dielectric films, and has led to the development of new device concepts such as resistive random‐access memory. Physical reconfigurability further allows memory and logic operations to be merged in the same device for efficient in‐memory computing and neuromorphic computing systems. By directly changing the chemical composition of the material, coupled electrical, optical, and magnetic effects can also be obtained. A survey of recent fundamental material and device studies that reveal the dynamic ionic processes is included, along with discussions on systematic modeling efforts, device and material challenges, and future research directions.