The distinct preferential alignment, i.e., horizontal orientation with respect to the substrate plane, of the optical transition dipole moment vectors (TDMVs) of organic dye molecules is of paramount importance for extracting the internally generated power of organic light-emitting diodes (OLEDs) to the outside world. This feature is one of the most promising approaches for the enhancement of the electrical efficacy in stateof-the-art OLEDs, as their internal quantum efficiencies are already close to the ultimate limit. If one can achieve complete horizontal orientation of the TDMVs, it is possible to increase the efficiency by at least 50% because alignment strongly influences the power dissipation into the different optical modes present in such a thin-film device. Thus, this feature of organic light-emitting molecules can lead to advanced performance for future applications. Therefore, we present here a review of recent achievements, ongoing research, and future tasks in this particular area of organic electronics.