Chiroptical Signal Inversion of Peptido‐Coassemblies in Confined Parallel‐Laminar Microfluidics

Abstract Chirality plays a vital role in material properties, and precise control of chiral signals is key to designing functional materials. Supramolecular self‐assembly offers an efficient means to integrate chiral building blocks with chromophores, yet controlling the assembly pathway remains challenging due to the complexity of non‐covalent interactions. Here, we introduce a continuous parallel‐laminar‐assisted self‐assembly strategy that exploits solvent ordering and solute diffusion in confined environments to regulate chiral signals in multi‐component peptide co‐assemblies. Notably, six nonpolar amino acids exhibit significantly enhanced chiroptical responses, as confirmed by circular dichroism (CD) and circularly polarized luminescence (CPL) spectroscopy. Intriguingly, Fmoc‐Ala and 1‐aminopyrene ( AP ) co‐assemblies formed in a microfluidic chip show a reversed chiroptical signal compared to those from batch reactions. Molecular dynamics (MD) simulations and COMSOL modeling suggest that velocity gradients and shear forces in microfluidics induce ordered non‐covalent interactions, altering excimer stacking and modulating chiroptical properties. This study presents an effective strategy for controlling chiral optical signals in confined environments, offering an interesting approach for supramolecular chiral transfer and regulation.