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21 × 106 and capacity of detecting CV molecules of concentrations as low as 10-10 M in their aqueous solutions. The growth mechanism of the anisotropic bimetallic nanostructures in DES and their SERS performance has been discussed. The simple DES-assisted synthesis strategy presented in this work can be adopted for large-scale nonaqueous fabrication of other bimetallic nanostructures in a quite "greener" way. Copyright © 2020 American Chemical Society.Two kinds of layered double hydroxide (LDH) Langmuir composite films containing azobenzene (Azo) groups wer