We report a vapor phase deposition method of high quality organic thin films, called molecular layer deposition (MLD). MLD is a gas phase process analogous to ALD and also relies on sequential saturated surface reactions which result in the formation of a self-assembled monolayer in each sequence. In the MLD method, the high quality organic thin films can be quickly formed with monolayer precision under ALD conditions (temperature, pressure, etc). The MLD method can be combined with ALD to take advantages of the possibility of obtaining organic–inorganic hybrid thin films. The advantages of the MLD technique combined with ALD include accurate control of film thickness, large-scale uniformity, excellent conformality, good reproducibility, multilayer processing capability, sharp interfaces, and excellent film qualities at relatively low temperatures. Additionally, a vast library of materials is accessible by ALD methods, ranging from single elements to compound semiconductors to oxides, nitrides, and sulfides. Therefore, the MLD method with ALD is an ideal fabrication technique for various organic-inorganic nanohybrid superlattices.