A critical requirement for the application of organic thin-film transistors (TFTs) in mobile or wearable applications is low-voltage operation, which can be achieved by employing ultrathin, high-capacitance gate dielectrics. One option is a hybrid dielectric composed of a thin film of aluminum oxide and a molecular self-assembled monolayer in which the aluminum oxide is formed by exposure of the surface of the aluminum gate electrode to a radio-frequency-generated oxygen plasma. This work investigates how the properties of such dielectrics are affected by the plasma power and the duration of the plasma exposure. For various combinations of plasma power and duration, the thickness and the capacitance of the dielectrics, the leakage-current density through the dielectrics, and the current–voltage characteristics of organic TFTs in which these dielectrics serve as the gate insulator have been evaluated. The influence of the plasma parameters on the surface properties of the dielectrics, the thin-film morphology of the vacuum-deposited organic-semiconductor films, and the resulting TFT characteristics has also been investigated.