Four-coordinate organoboron compounds with rigid π-conjugated structures are intensely luminescent and have high carrier mobility which enables them to be applied in optoelectronics including organic light-emitting diodes (OLEDs), organic field-effect transistors, as well as photoresponsive, sensory and imaging materials. Various chelate ligands and boron moieties have been explored to construct proper electronic structures and suitable molecular arrangements, which play important roles on the photophysical and electronic properties of the four coordinate boron compounds. These efforts have produced a number of fascinating molecules, some of which have exhibited high performance as light emitting materials. In this article, we provide an overview of the progress in the molecular construction of four-coordinate organoboron compounds with an emphasis on their applications in OLEDs.