Multifunctional ionic plastic crystals (IPCs) are a class of unique materials that exhibit a wide range of advanced applications. In this work, we proposed a strategy for the design of multifunctional, superior ion-conducting IPCs with bistability in both magnetic and electric properties, moreover, we successfully prepared and thoroughly characterized such an IPC, [PMPyr][Ni(mnt)2] (1; PMPyr+=N-propyl-N-methylpyrrolidinium, and mnt2-=maleonitriledithiolate). Plastic crystal 1 exhibits superior ion conduction near room temperature, and its ion conductivity reaches the order of 10-2 S cm-1 at 373 K. Remarkably, the crystal-to-plastic crystal transformation results in 1 simultaneously exhibiting electrical bistability and magnetic transition. Our study paves the way for the development of new IPCs with desirable functional properties.
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