Coordinated ionic liquid (IL) monomers provide many of the benefits of conventional ILs in radical polymerization with the advantage of relatively simple synthesis and recovery of the polymer product. Previous studies have reported high solubilities of lithium bistriflimide in polar organic monomers such as methyl methacrylate (MMA), 1‐vinylimidazole (VIm) and others. Here, coordinated IL monomers are formed comprising a variety of alkali and alkaline earth Mn+(Tf2N−)n salts with MMA and VIm, and polymerization behavior is investigated using real‐time attenuated total reflectance Fourier transform infrared spectroscopy (ATR FT‐IR). The size and valency of the coordinated Mn+ cations are observed to strongly influence monomer reactivity, as evidenced by significant changes in FT‐IR spectra. This work further demonstrates that the bulky, delocalized [Tf2N]− anion allows for facile introduction of a wide range of Mn+ cations into organic polymers without phase separation, which may open opportunities for new composite materials.

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