The present doctoral thesis aims to contribute to the field of organic semiconductor physics and technology, both of which have become fast growing disciplines. Two technological applications are emerging from these research efforts: Organic light-emitting diodes (OLEDs) and organic field-effect transistors (OFETs). OLEDs are already being fabricated on an industrial level today, while some fundamental issues still remain to be resolved for OFETs. During the last ten years, research interest has been continuously shifting from the bulk properties of organic semiconductors to their interfaces. Such issues are in fact addressed in this thesis work and include different interactions of thin organic layers with their environments. In the field of OLEDs, a multitude of issues have been investigated here. Most importantly and in contrast to most publications in this field, OLED's with complex device architectures that fully compete with standard devices performancewise have been fabricated and characterized. An oxygen plasma treatment of indium-tin-oxide anode has been shown to reduce the injection performance while enhancing the quantum efficiency. Two different mechanisms are proposed to explain this. Going a step further, the life-time behavior of such devices has been examined. Different aging mechanisms were identified: in short term and intermediate term aging, an oxygen plasma treatment of anode clearly reduces the operational voltage. Bulk degradation of the organic electroluminescent layer then becomes predominant for long term aging. Another important finding concerns the formation of exciplexes at organic/organic heterojunctions: In devices comprising a high hole injection barrier between the hole-transport and the electron-transport layer, the dominant formation of exciplexes is identified by a red-shifted shoulder in the electroluminescent spectrum and a low quantum yield. In contrast to that, the quantum efficiency is increased markedly by minimizing this hole barrier. In such devices, the formation of exciplexes is beneficial for device performance, since it facilitates hole transfer across the heterojunction. For the first time, the operational currents could be divided into different radiative and non-radiative recombination channels of exciplexes and excitons respectively. This quantification was further developed to simulate current-versus-voltage behavior and quantum efficiency. The work on pentacene based devices was initiated by fabricating ultrathin pentacene films on polished sapphire and by characterizing them with a temperature variable four probe setup. Oxygen plasma treatment of the substrate introduces oxygen radicals onto the surface and subsequent pentacene deposition leads to electron extraction from the pentacene molecules to defects at the oxide surface. Such an increase of charge carrier density within the semiconducting layer enhances its conductivity. Using a thick, aliphatic self-assembled monolayer (SAM) as an intermediate layer, both the activation energy and the film resistance increase by at least an order of magnitude compared to devices without SAM. Hence, charge transfer to the substrate is inhibited. The OFETs fabricated for this thesis work are all based on pentacene as a semiconductor and the gate interface was the focus of interest. Two different device types were fabricated: One device category comprises ultra-thin film OFETs (10nm). In such devices contact resistance is negligible. This gives rise to a dependence of device behavior on the gate interface. For this reason, the dielectric constant of the gate insulator was varied by changing the gate materials: the hole mobility is enhanced four-fold by using an aliphatic SAM at the gate interface instead of an oxygen plasma treated alumina (Al2O3). This effect has been interpreted in terms of self-trapping at the interface and its reduction by a low-k dielectric gate. In addition the on-off ratio was enhanced by a factor of 20, thanks to the SAM-inhibited pentacene doping due to a reduced semiconductor/substrate interaction. The second OFETdevice category was based on thicker (80nm) pentacene films. Their behavior is injection controlled. This finding originates in the application of a top contact configuration which implies that the carriers cross the granular material to reach the channel. Impedance spectroscopic measurements on different metal-insulator-semiconductor diodes unveiled a morphology dependent transveral mobility, which is linked to the degree of structural disorder in the film. In conclusion: Understanding of the various physical processes occurring at the different interfaces (anode and organic/organic interfaces in OLEDs, gate interface in OFETs) has considerably improved the performance of organic semiconductor based devices.