EDT-TTF-CONHCatOH, a catechol-appended TTF derivative, 5 was synthesized through a straightforward strategy. The electronic absorption and the electrochemical investigations as well as molecular orbital calculations for compounds 4 and 5 have been performed. The electrochemical measurements of 5 indicate that it is a suitable candidate for the formation of zwitterionic molecular solids and also two-component radical cation salts. The crystal structure of compound 5 reveals supramolecular dimers assembled via a set of O-H center dot center dot center dot O hydrogen bonds between the catechol and amide units.