Bimetallic and multimetallic intramolecular charge-transfer compounds have been widely studied electrochemically to reveal information on metal-metal interactions mediated by π-conjugated ligands. We present recent experimental and theoretical studies on a series of Ru-containing oligomers and polymers for use as molecular wires. These results suggest that conjugated π-bridged metal oligomers can exhibit extremely low band gaps, greater delocalization than conventional organic conjugated polymers, and easily-tailorable electronic structure properties via ligand and metal substitution. Beyond bulk electrochemistry and spectroscopy, single-molecule transport measurements are discussed.