Global Chirality in Pillar-Layered Metal-Organic Frameworks Amplifies Circularly Polarized Luminescence

• • The |g_lum| values of the pillar-layered MOFs are amplified by up to 23-fold compared to free ligands, reaching levels comparable to state-of-the-art chiral assemblies, enabling high-purity CPL for display and security applications. • • Photoluminescence quantum efficiencies (Φ_PL) reach up to 67%, a ~34-fold increase over free ligands, demonstrating that structural rigidification in MOFs effectively suppresses aggregation-caused quenching, crucial for solid-state lighting and bioimaging. • • The CPL activity arises from global chirality of the hierarchical framework, not the intrinsic chirality of precursors, providing a general design principle for chirality transfer in extended porous materials. • • The co-assembly of enantiopure R/S-binol with achiral luminescent ligands yields three pairs of enantiomeric pillar-layered MOFs, showcasing the versatility of chiral reticular chemistry for creating homochiral frameworks with tunable photonic properties.