Organic electronics is the technology enabling truly flexible electronic devices. However, despite continuous improvements in the charge-carrier mobility, devices used for digital circuits based on organic field-effect transistors (OFETs) have still not achieved a commercial breakthrough. A substantial hurdle to the realization of effective digital circuitry is the proper control of the threshold voltage V_th. Previous approaches include doping or self-assembled monolayers to provide the threshold voltage control. However, while self-assembled monolayers-modified OFETs often do not show the level of reproducibility which is required in digital circuit engineering, direct doping of the channel material results in a poor on/off ratio leading to unfavorable power dissipation. Furthermore, direct doping of the channel material in organic semiconductors could cause the formation of trap states impeding the charge-carrier transport. Employing the concept of modulation-doped field-effect transistors (MODFETs), which is well established in inorganic electronics, the semiconductor− dopant interaction is significantly reduced, thereby solving the above-described problems. Here, we present the concept of an organic semiconductor MODFET which is composed of an organic−organic heterostructure between a highly doped wide-energy-gap material and an undoped narrow-energy-gap material. The effectiveness of charge transfer across the interface is controlled by the doping concentration and thickness of an undoped buffer layer. A complete picture of the energy landscape of this heterostructure is drawn using impedance spectroscopy and ultraviolet photoelectron spectroscopy. Furthermore, we analyze the effect of the dopant density on the charge-carrier transport properties. The incorporation of these heterostructures into OFETs enables a precise adjustment of the threshold voltage by using the modulation doping concept.