Understanding and controlling the driving forces for molecular alignment in optoelectronic thin-film devices is of crucial importance for improving their performance. In this context, the preferential orientation of organometallic iridium complexes is in the focus of research to benefit from their improved light-outcoupling efficiencies in organic light-emitting diodes (OLEDs). Although there has been great progress concerning the orientation behavior for heteroleptic Ir complexes, the mechanism behind the alignment of homoleptic complexes is still unclear yet. In this work, we present a sky-blue phosphorescent dye that shows variable alignment depending on systematic modifications of the ligands bound to the central iridium atom. From an optical study of the transition dipole moment orientation and the electrically accessible alignment of the permanent dipole moment, we conclude that the film morphology is related to both the aspect ratio of the dye and the local electrostatic interaction of the ligands with the film surface during growth. These results indicate a potential strategy to actively control the orientation of iridium-based emitters for the application in OLEDs.