Training‐Augmented Ionic Switch for Logic Signal Modulation

Abstract Efficient ionic conductivity switching is crucial for the progression of iontronics, where adaptability and dynamic control are desirable to the innovation of intelligent devices. One of the main challenges in the field is to develop materials that not only transit between distinct conductive states but also exhibit evolvable properties to enhance their functional capabilities. Addressing this, a reversible phase‐transition hydrated salt crystal ionic gel (RPSIG) for innovative ionic switch design is introduced. The RPSIG demonstrates an exceptional ability to modulate its ionic conductivity, with a switching ratio able to reach 5000‐fold after training. The training effect can be attributed to the enhanced synergistic interplay between crystallites and the polymer matrix, which leads to thermodynamic stabilization of the interfacial structure and induces a higher energy cost for ion migrations. Meanwhile, the RPSIG exhibits the capability to adjust its resistive‐capacitive properties in response to phase transitions, making it a versatile component for signal processing. Further application of RPSIG in intelligent latches and multifunctional hybrid circuits enables effective logic signal transmission, highlighting its potential in pioneering the development of advanced iontronic devices.