Molecular electronics has been considered a beyond-CMOS platform to pursue the scaling of electronic devices, by pushing it to the single-molecule level, and by using the paradigm in which individual molecules constitute the active components in electronic circuits, performing a variety of functions such as transistors and sensors. For many years, molecular electronics has traditionally advanced from materials such as gold electrode with nanogap formation methods such as electromigration and mechanical break junctions. Alternatively, graphene has opened a new possibility of acting as a stable electrode at room temperature for a long period of time and its unique electronic properties have been analyzed as a possible material to be the electrode for single-molecule electronics.