A method is provided for fabricating molecular electronic devices comprising at least a bottom electrode and a molecular switch film on the bottom electrode. The method includes forming the bottom electrode by a process including: cleaning portions of the substrate where the bottom electrode is to be deposited; pre-sputtering the portions; depositing a conductive layer on at least the portions; and cleaning the top surface of the conductive layer. Advantageously, the conductive electrode properties include: low or controlled oxide formation (or possibly passivated), high melting point, high bulk modulus, and low diffusion. Smooth deposited film surfaces are compatible with Langmuir-Blodgett molecular film deposition. Tailored surfaces are further useful for SAM deposition. The metallic nature gives high conductivity connection to molecules. Barrier layers may be added to the device stack, i.e., Al2O3 over the conductive layer.