circular dichroism, [3] electronic circular dichroism [4] and Raman optical activity, [5] has been used in both quantitative analysis and absolute configuration study of the enantiomers. However, the feasibility of enantiomeric discrimination by chiral chromatography strongly depends on molecular polarity and mass of enantiomers, which narrows applicable conditions and molecules for each chiral column. Chiral spectroscopy is impossible to be used for enantioselective discrimination of racemates or chiral molecules with inherently weak optical response suffering from poor resolution and low sensitivity. [6] Recently, we developed new strategies, PM-ChA [7] and SERS-ChA [8] of chiral nanostructured Au films (CNAFs) to enantiomers, which demonstrated enantiomeric determination, based on the selective generation of photomagnetic fields (PMFs) and selective enhancement of Raman scattering of enantiomeric molecules on CNAFs, respectively. These methods are available for all the enantiomers regardless of their sizes, polarities, or chromophores, which overcome the drawbacks of chromatography and spectroscopy.Silver (Ag) nanomaterials show strong SPR effects and excellent electrical conductivity, making them promising for plasmonic sensing systems and optoelectronic devices. [9] Therefore, doping with Ag should allow modulating the SPR and increasing conductivity of composite nanomaterials, which is expected to generate stronger local electromagnetic fields and further enhance the SERS intensities. This strategy provides the possibility for simultaneous enhancement of the PM-ChA and SERS-ChA effects of chiral noble metal nanomaterials. However, multi-metal compounding by the wet chemical deposition method sometimes suffers from difficulty in finding a reductant with appropriate reducing potential for simultaneous codeposition of metal ions in the precursor solution.Electrodeposition is a universal, efficient, and low-consumption technique for the preparation of Ag containing composite nanomaterials comparing with the other methods, [10] because deposition occurs in a very limited range on the electrode surface and the electrodeposition method allows precisely controlled reduction potential and duration time for Ag material preparation. [11] In addition, reduction reaction rates of different metal ions can be adjusted by changing the reduction potential, which makes them uniformly deposited Herein, the chiral nanostructured bimetallic Au-Ag films (CNAAFs) with both photomagnetic-chiral anisotropy to enantiomers (PM-ChA C-E ) and surface-enhanced Raman scattering-chiral anisotropy to enantiomers (SERS-ChA C-E ) for efficient enantiomeric discrimination are reported. The CNAAFs are synthesized by electrodeposition on n-type Si (n-Si) substrates with the assistance of N-acetyl-L/D-cysteine (S/R-NAC) as symmetry-breaking agents, which are consisted of polycrystalline Boerdijk-Coxeter-Bernal (BCB) tetrahelical structured Au-Ag alloy nanowires grown on n-Si substrates perpendicularly. The anisotropic factors of PM-ChA C-E ...