In this paper, organic thin film transistors with different configurations are fabricated, and the effect on their performance when tailoring the semiconductor/insulator and semiconductor/contact interfaces through suitable treatments is analyzed. It is shown that the admittance spectroscopy used together with a properly developed electrical model turns out to be a particularly appropriate technique for correlating the performance of devices based on new materials in the manufacturing methods. The model proposed here to describe the equivalent metal–insulator– semiconductor (MIS) capacitor enables the extraction of a wide range of parameters and the study of the physical phenomena occurring in the transistors: Diffusion of mobile ions throu...