The preparation of the homoleptic MM quadruply bonded complexes Mo-2(O2CC6H4-p-X)(4), where X = (I) or C equivalent to N (II), is reported along with the solution characterization data and electronic structure calculations employing density functional theory. The compounds are colored orange (I) and red (II) due to the metal-to-ligand charge transfer involving the HOMO, Mo-2 delta, and LUMO, which is a ligand-based pi* combination. Studies of the S, state, (MLCT)-M-1, by femtosecond time-resolved infrared spectroscopy indicate that the negative charge is distributed principally over two trans ligands. The T, states are Mo-3-Mo delta delta* as determined by NIR emission and nanosecond transient absorption.