Nascent molecular electronic devices, based on monolayer Langmuir–Blodgett films sandwiched between two carbonaceous electrodes, have been prepared. Tightly packed monolayers of 4‐((4‐((4‐ethynylphenyl)ethynyl)phenyl)ethynyl)benzoic acid are deposited onto a highly oriented pyrolytic graphite electrode. An amorphous carbon top contact electrode is formed on top of the monolayer from a naphthalene precursor using the focused electron beam induced deposition technique. This allows the deposition of a carbon top‐contact electrode with well‐defined shape, thickness, and precise positioning on the film with nm resolution. These results represent a substantial step toward the realization of integrated molecular electronic devices based on monolayers and carbon electrodes.