Electrification of thermal chemical processes could play an important role in creating a more energy efficient chemical sector. Here we demonstrate that a range of MLC catalysts can be successfully electrified and used for imine formation from alcohol precursors, thus demonstrating the first example of molecular electrocatalytic C–N bond formation.This novel concept allowed energy efficiency to be increased by an order of magnitude compared to thermal catalysis. Molecular EAO and the electrification of homogeneous catalysts can thus contribute to current efforts for the electrocatalytic generation of C–N bonds from simple building blocks.