monoammonium‐based organicelectrolytes with the tetrafluoroborate (BF4−) counteranion have been synthesized. Replacing the pendant ethyl groups in the fluorenyl unit with 4‐ethoxyphenyl groups dramatically improves both solubility and morphological stability. The characterization of the alcohol‐processable amorphous ionic compounds as an electron‐injection layer in organic light‐emitting diodes (OLEDs) reveals