Graphene, as a monolayer of graphite, has an ultra-high Young’s modulus of ~1 TPa, which makes it a promising candidate for Nano-Electromechanical (NEM) devices. The graphene NEM switches is expected to show minimized electrical leakage, sharp switching response, low actuation voltage, and high on/off ratio. A simple bottom-up procedure using a polymer sacrificial spacer is utilized to fabricate graphene electromechanical contact switch devices. Low pull-in voltage of below 5 V is achieved with good consistency [1], which is compatible with the conventional complementary metal-oxide-semiconductor circuit requirements. In addition, the formation of carbon-gold bonds at the contact position is proposed as another important mechanism for the irreversible switch other than the well-known irreversible static friction. In order to overcome the stiction issue and realize repetitive switching operations, we exploited a natural chromium oxide layer formed on the chromium electrode. We fabricated a doubly-clamped beam and cantilever graphene nanoelectromechanical switches with a local top actuation electrode. The low pull-in voltage below 5 V was realized in both of the switches. The naturally formed chromium oxide at the graphene-electrode contact interface prevents the formation of chemical bonds between graphene and metal, resulting in reversible switching operation successfully. Thanks to highly-stable SP2 bonds in a 2D honeycomb lattice, graphene exhibits an extremely suppressed electrical noise, making it possible to realize extremly-sensitive sensor. For the physisorbed CO2 molecules - graphene vdW complexes, we found it is possible to tune the vdW interaction with external electric fields. The field-dependent charge transfer in the CO2−graphene complex was unveiled along with small variations in the equilibrium CO2−graphene distance and the O−C−O bonding angle. By reversing the substrate bias polarity, the charge transfer direction also switched, signifying the role of physisorbed CO2molecules can be altered electrically between donor and acceptor. The range of such electrical tunability was found inherent in individual molecular species [2]. In recent years, direct milling of graphene by Helium ion beam (HIB) has been actively explored. The main advantages of HIB milling over typical gallium focused ion beam (FIB) milling are: high resolution and less damage to the graphene. This HIB milling can be actively explored to carve the suspended graphene into a very narrow beam, which will help to realize narrower suspended graphene beams, which can’t be realized with the standard electron beam lithography technique. Towards this direction, gas field ionization source (GFIS) system with Helium and Nitrogen beams is introduced. In order to use HIB milling, a suspended monolayer graphene beam device was first fabricated without a top gate. These devices were used for the further HIB milling. We successfully patterned a 60-nm-long and 15-nm wide suspended graphene beam. As the next step to utilize our unique graphene nano-electro-mechanical systems (NEMS) to realize a well challenging application, the NEMS sensor devices were explored to realize individual CO2 molecule detection. Detection of a single molecule’s adsorption and desorption, which determines the ultimate resolution of gas sensing, has rarely been achieved with conventional solid-state sensor devices. A doubly clamped bilayer graphene beam was first fabricated and then by applying a voltage to the lower gold electrode the graphene beam was electrostatically pulled down. It was found that despite the negligible charge transfer from a single very poor doping CO2 physisorbed molecule, it strongly affects the electronic transport in suspended graphene beam by inducing charged impurity, which can shut down part of conduction of the graphene channel with Coulomb impurity scattering. We detected each individual physisorption of CO2molecule as a step-wise resistance change with a quantized interval for the graphene channel [3].