Since several years ago, supramolecular chemistry, in general, has become one of the challenges for materials science, including the synthesis of new supramolecular materials and the production of the new supramolecular arrangements using thin film deposition techniques. Once the supramolecular arrangement is a crucial factor in achieving excellent device performance, the development of novel sensor systems is one of the most promising fields of supramolecular chemistry. In this chapter, we focus on the developments in supramolecular thin films applied to sense applications. We bring a brief overview of three different techniques to thin film deposition, Langmuir based (Langmuir–Blodgett and Langmuir–Schaefer), electrodeposited, and Layer-by-Layer films. Some examples of tuning supramolecular arrangements and their effects on the sensor's performance were also described.