Magic-sized clusters (MSCs) are nanomaterials with discrete electronic properties, ideal for photonic and optoelectronic applications. This thesis investigates the structure of mesophase CdS and CdSe MSCs and their chiral self-assembly in thin films. First, we examined the self-assembly of CdS MSCs into hierarchical films, achieving macroscopic homochiral domains with significant circular dichroism through controlled evaporation. Next, we synthesized and generated CdSe MSC films, demonstrating the robustness of this chiral self-assembly method across different MSC systems. Additionally, we briefly explored the design and fabrication of chiral-induced spin-selective (CISS) magnetic tunnel junctions by intercalating chiral molecules into 2D superlattices. Collectively, these studies advance the understanding of chiral self-assembly in nanomaterials, paving the way for future innovations in nanotechnology.