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Ionic liquid (IL)‐containing polymers garner attention for electrochemical applications. This article overviews recent experimental and theoretical studies of polymer electrolytes that would be likely to cultivate new theoretical and computational frameworks for IL‐containing polymers. The first two sections outline the uniqueness of ILs that differentiates them from inorganic salts in polymers and explore deviation from the concept of the metaphor “room‐temperature molten salt.” Such distinct properties include (1) large intrinsic dipole moment and electronic polarizability, (2) hydrogen bonding, (3) π‐interactions, (4) a broad distribution of charges over the entire ion, and (5) the anisotropy of the ions. Moreover, the complexity of these properties substantially increases when the ions are polymerized. Indeed, their exceptional features would overcome the hurdle due to a trade‐off between ionic conductivity and mechanical robustness in inorganic salt‐doped polymers. Given these facts, the rest of the article focuses on emerging trends in the study of the dielectric response, phase separation, ion conductivity, and mechanical robustness of the polymer electrolytes, highlighting outstanding observations in experiments that may inspire existing theory and simulation. Our discussion also includes improving computational complexity for IL‐containing polymers. To this end, recent machine learning studies that consider ILs and polymer liquids are presented.

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