Interaction-structure coupling enables high-flux enantioselective transport in lamellar membranes.

Enantioselective transport in solid membranes is often limited because weak stereospecific interactions are difficult to translate into substantial kinetic discrimination under fast diffusion. Here we show that such weak recognition can be amplified through an interaction-structure coupling mechanism in lamellar membranes. Helical ssDNA-wrapped single-walled carbon nanotubes were intercalated into graphene oxide laminates to construct continuous chiral transport pathways with adaptive confined interfaces. Opposite phenylalanine enantiomers induce distinct reconfiguration of the lamellar galleries, leading to differentiated interlayer spacings and a pronounced split in apparent migration barriers. After reduction, the resulting membrane exhibits a large activation-energy difference between l- and d-phenylalanine transport, enabling high-flux enantioselective permeation, separation factors up to 12.59, stable operation over 168 h, and cascade enrichment to 99.95% of l-phenylalanine optical purity. These results establish interaction-structure coupling as an effective strategy for amplifying subtle molecular recognition into robust transport selectivity in confined membrane systems.