The precise fabrication of nanostructured materials on surfaces is paramount for advancing next-generation technologies in catalysis, electronics, biomedicine, etc. Recently, surface-initiated living crystallization-driven self-assembly (SIL-CDSA) has enabled unprecedented control over the architecture, orientation, and functionality of solid-state nanostructures on desired substrates. This review outlines key principles of SIL-CDSA, including seed immobilization, confined epitaxial growt