The use of vibrational spectroscopy in characterizing synthetic organic superconductors is reviewed. The electron-donor molecules tetramethyltetraselena-fulvalene (TMTSF) and bis(ethylenedithio)tetrathia-fulvalene (BEDT-TTF or ET), which provide superconducting salts when combined with anions, are highlighted. Special emphasis is given to the microreflectance technique and its usefulness in the study of these materials.