The effective work functions of both metal and metal oxide electrodes, intended for use as contacts to organic thin films in organic electronic devices, are critically affected by the surface composition of the contact. Interface dipoles can be routinely expressed at the surface of a metal electrode, such as Au, using various self-assembled monolayers, with either high or low electron affinity terminal functional groups. We have recently shown that the effective work function of a gold electrode, as probed by UV-photoelectron spectroscopy, can be smoothly altered by over 1.5 eV using various combinations of alkanethiols. In the case of metal oxides, such as ITO, the situation heretofore has been more complicated, owing to the fact that the modifiers attach primarily to ultra-thin, electrically passive layers over the conducting bulk oxide (as revealed by our recent C-AFM studies of acid-etched and freshly deposited ITO). Our recent attempts at chemical modification of freshly deposited ITO films, their in vacuuo modification, and the effects of these modifications will also be reviewed in this talk.