In this paper, we report on the syntheses, structures, and characterization of four molten salts containing imidazolium cations and europium(III)- or terbium(III)-centered complex anions. In the complex anions, the lanthanide centers are wrapped by four pseudodiketonate anionic ligands, which prevent them from contacting with high-frequency oscillators and allow them to show intense characteristic europium(III) or terbium(III) emission, small line widths, high color purity, high quantum yields (30−49%), and long decay times (>2 ms).