Researches in both, academia and industry are investigating optical loss channels in OLED layered systems by means of optical simulation tools in order to derive promising concepts for a further enhancement of the overall device performance. Besides other factors, the prospects of success of such optimization strategies rely severely on the credibility of the optical input data. The present thesis provides a guideline to measure the active optical properties of OLED emitter materials in situ by radiation pattern analyses. Reliable and widely applicable methods are introduced to determine the internal electroluminescence spectrum, the profile of the emission zone, the dipole emitter orientation, and the internal luminescence quantum efficiency of emissive materials from the optical far field emission of OLEDs in electrical operation. The proposed characterization procedures are applied to sets of OLEDs containing both, fluorescent polymeric materials as well as phosphorescent small-molecular emitters, respectively. On the one hand, quite expected results are obtained. On the other hand, several novel and truly surprising results are found. Most importantly, this thesis contains the first report of a non-isotropic, mainly parallel emitter orientation in a phosphorescent small-molecular guest-host system (Ir(MDQ)2(acac) in a-NPD). Due to the latter result, emitter orientation based optimization of phosphorescent OLEDs seems to be within reach. Since parallel dipoles emit preferably into air, the utilization of smart emissive materials with advantageous molecular orientation is capable to boost the efficiency of phosphorescent OLEDs by 50%. Materials design, the influence of the matrix material and the substrate, as well as film deposition conditions are just a few parameters that need to be studied further in order to exploit the huge potential of the dipole emitter orientation in phosphorescent OLEDs.