For the design and manufacture of complex integrated circuits, control over the threshold voltage of the transistors is essential. In the present contribution, we present a non-invasive method to tune the threshold voltage of organic thin-film transistors after device assembly over a wide range without any significant degradation of the device characteristics. This is realized by incorporating a thin, chemically reactive siloxane layer bonded to the gate oxide. This results in threshold voltages of around 70 V in the as-prepared devices. By exposing a transistor modified in this way to ammonia at different concentrations, the threshold voltage can be tuned in steps of only a few volts. This treatment affects only the charge density at the semiconductor-dielectric interface, leaving the overall shape of the transistor characteristics and the charge-carrier mobility largely unaltered.