A new series of cationic blue-emitting, heteroleptic indium(III)-based metal complexes were systematically synthesized using two 4,6-difluorophenylpyridine ligands as well as one methyl- or n-butyl-substituted bisimidazolium salt carbene-type ligand. In degassed CH2Cl2, all complexes display highly efficient, blue phosphorescence (lambda(max) similar to 452 nm; emission quantum yield similar to 0.30) at room temperature and also show blue emission in a thin film. The measured photophysical properties of the complexes have been rationalized with the help of quantum-chemical calculations. Because of the high solubility of the complexes, solution-processed devices, light-emitting electro-chemical cells (LEECs), were made. The results showed that true blue emission and short turn-on time is achieved when an ionic conductor, tetrabutylammonium trifluoromethanesulfonate, was used as the matrix for the film containing the emitters. These iridium complexes and the described devices are the bluest materials ever reported and the first case of LEECs based on carbene ligands.