Forged signature threatens the authenticity of personal identity. Here, an effective SERS anti-counterfeiting system is designed for personal signatures. Mixed ligands improve the complexity of Raman spectra and expand the coding capacity. Fourteen distinct combinations are created from mere five ligands, and great expansion is possible with modest expansion of the ligand library. On the other hand, the (Au-aggregate)@Ag@PSPAA nanostructure significantly increases the surface-enhanced Raman scattering (SERS) intensity and stability so that excellent performance is achieved in SERS detection. By integrating these strategies, SERS inks are produced and applied in signature anti-counterfeiting. The resulting spectra are converted to barcodes that are readily detected through a smart phone APP. With these improvements, this work brings SERS one step closer toward practical applications in signature anti-counterfeiting.