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Understanding the morphology of organic materials within optoelectronic thin film devices is of crucial importance for the development of state-of-the-art organic light emitting diodes (OLEDs). In this context, the preferential alignment of organometallic Ir complexes has been in the focus of research to benefit from the improved light-outcoupling efficiencies. Although the emissive dipole orientation has been identified from an optical point of view and molecular dynamic simulations give first insights into film morphologies, new experimental techniques are necessary to pinpoint the exact alignment of phosphorescent dye molecules. In this work, optical characterization of luminescent thin films was combined with electrical measurements on bilayer devices to elucidate the orientation distribution of both, electrical and optical dipole moments of phosphorescent guest–host systems. The results not only confirm previous suggestions for the alignment mechanism of organometallic dyes but also disclose a direct correlation between the degree of electrical and optical dipole alignment, thus opening a roadway for achieving higher light-outcoupling efficiency in OLEDs.