Chiral semiconductors combine the merits of asymmetrical geometry and semiconductors, exhibiting selectivity for light (left-handedness/right-handedness) and electrons (spin up/spin down). These materials show great potential for developing energy-efficient and durable optoelectronic devices, including light-emitting diodes, solar cells, and photodetectors. Understanding and establishing structure-property correlations of chiral semiconductors, from molecular to microscopic levels, will create opportunities for the innovation of optoelectronic devices. In this talk, I will showcase how my research integrates diverse synthesis methods, versatile chemical designs, multimodal material characterization, and proof-of-concept devices to advance chiral semiconductors for optoelectronics. I will first focus on introducing the spontaneous self-assembly phenomenon and structure-chiroptical relationship of chiral CdSe/CdS nanorods and their assemblies, as well as their application in light-emitting diodes for generating circularly polarized light. I will also demonstrate how to leverage the geometric advantages of chiral perovskites to enhance the mechanical properties of critical interfaces in perovskite solar cells. In this context, I will further discuss the challenges and opportunities associated with chiral semiconductors and highlight the broader interest in chiral materials.