The generation and amplification of chirality in inorganic nanomaterials have garnered significant attention due to their promising applications in enantioselective catalysis, chiral sensing, and optoelectronics. Interface-driven self-assembly has emerged as a robust and versatile strategy to induce and enhance chirality in these systems, offering precise control over the spatial organization of nanoscale building blocks. This review presents a comprehensive overview of recent advancements in interface-driven self-assembly techniques, focusing on how these methods facilitate the generation and amplification of chiroptical properties in inorganic nanomaterials. We examine the strategies of interface-driven self-assembly through external torsion, aggregation amplification, and chiral molecule induction, highlighting key mechanisms that contribute to enhanced chiral responses. Self-assembly processes at liquid–liquid, gas–liquid, and liquid–solid interfaces are critically discussed, along with the influence of parameters, such as nanoparticle shape, surface ligand composition, and external stimuli on the formation of chiral nanostructures. Additionally, theoretical models describing the emergence of chirality are examined, providing insights into the role of interfacial molecular interactions in driving observed chiroptical effects. Finally, we review the applications of these chiral nanomaterials in spintronics, chiral photonics, and beyond, and propose future directions for advancing the design and development of novel chiral inorganic nanomaterials. This robust strategy holds great potential for facilitating breakthroughs in both the fundamental understanding and the practical implementation of chiral nanostructures.