Highly-oriented polycrystalline thin films of molecular organic materials consisting of small molecules can be easily obtained by physical and chemical vapour deposition methods. The crystallographic phase, orientation and morphology of the films critically depend on the interface and on the kinetics of growth and can be controlled, to a certain extent, by a judicious selection of the substrates and of the growth parameters. This article shortly explores the formation of organic-inorganic heterostructures as a function of coverage: from the most fundamental case, a single molecule on a surface, to thick films (thickness 1 μm). The case of high-quality thick TTF-TCNQ films exemplifies the fact that the derived physical properties are essentially identical to those obtained from single crystals.