The combination of inorganic and organic semiconductors in a heterojunction is considered a promising approach to overcome limitations of each individual material class. However, to date only few examples of improved (opto-)electronic functionality have been realized with such hybrid heterojunctions. The key to unraveling the full potential offered by inorganic/organic semiconductor heterojunctions is the ability to deliberately control the interfacial electronic energy levels. Here, a universal approach to adjust the offset between the energy levels at inorganic/organic semiconductor interfaces is demonstrated: the interlayer method. A monolayer-thick interlayer comprising strong electron donor or acceptor molecules is inserted between the...