We report the synthesis of cationic 2,6-bisiminopyridine organoaluminum complexes, [(BIP)AlR2]+, as stable BArF4- or PF6- salts, and their reversible single-electron reduction into well-defined paramagnetic species, [(BIP·)AlR2]. Four redox couples, [(BIP)AlR2]+/0, have been fully characterized through structural, spectroscopic, electrochemical and computational techniques.