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Films based on poly(vinylidene fluoride) (PVDF) blended with ionic liquids (ILs) comprising different cations and anions were developed to investigate the IL influence on the resulting PVDF crystalline phase. Blends with 25 wt % IL content were produced by solvent casting followed by solvent evaporation at 210 °C in an air oven. Five different ILs containing the same cation 1-ethyl-3-methylimidazolium [Emim] and five ILs containing the same anion bis(trifluoromethylsulfonyl)imide [TFSI] were selected. The formation of the different phases and the resulting thermal and dynamic mechanical properties were studied by Fourier transform infrared spectroscopy, differential scanning calorimetry, and dynamic mechanical analysis. The incorporation of [Emim]-based ILs successfully directs the PVDF crystallization from the nonpolar α-phase toward the electroactive and highly polar β-phase. On the contrary, blends containing [TFSI] as a