The synthesis of the first examples of cyano-substituted low-symmetry ball-shaped ruthenium complexes is reported. Systematic mixed condensation reactions of benzonitrile, terephthalonitrile, 1,3-diiminoisoindoline, and a ruthenium salt afforded ball-shaped complexes that contain zero to four cyano groups. The absorption spectra of these complexes revealed that the red to NIR band was blue-shifted and that the visible band was red-shifted with increasing number of cyano groups. The substituent effect of the number of cyano groups was rationalized based on theoretical calculations.