Counterfeiting is a global longstanding problem that causes significant negative impact on a wide range of products from banknotes, valuable documents, medicine, luxury to common consumer goods, endangering the economy, safety, and human health, etc. [1][2][3][4] A variety of anticounterfeiting techniques have been developed, such as those based on hologram, watermarks, radio-frequency identification, structural color, graphic code, molecular tag, physical unclonable, fluorescence, surface-enhanced Raman scattering (SERS), and so on. [5][6][7][8][9][10][11][12][13][14][15][16][17][18][19] The actual benefits and practicality of the anticounterfeiting techniques are strongly affected by comprehensive factors including the safety index, capacity, stability, readability, manufacturing, and cost, etc. Each anticounterfeiting technique has its own advantages and limitations, as shown in Figure S1 in the Supporting Information, and to fit all the required factors mentioned above remains a great challenge. [5][6][7][8][9][10][11][12][13][14][15][16][17][18][19] Considering the most important parameter-encoding capacity, the two molecular tag [15,16,19] and SERS [5,6,[19][20][21] anticounterfeiting techniques related to molecular information and the physical unclonable technique related to the spatial random distribution of the particles, which are difficult to forge and have a higher tolerance to errors, show great advantages. Compared with fluorescence labels, SERS labels can be verified by SERS spectra with narrower fingerprint bands under the excitation at different wavelengths; [22][23][24] moreover, SERS labels exhibit superior photostability due to the extremely short lifetimes of Raman scattering which can inhibit photo-bleaching, energy transfer, or quenching of the probe molecules in the excited states. [6,[22][23][24][25] In general, among the various anticounterfeiting techniques, SERS-based anticounterfeiting stands out in recent years, not only due to its higher information capacity and higher safety index, but also due to its excellent comprehensive performance. [20,21] Raman scattering, resulting from the vibrational signatures of molecules, was discovered in the 1920s by the Indian physicist C.V. Raman. [26,27] In recent years, SERS has become a commonly used sensing technique in various fields including anticounterfeiting, in which inelastic light scattering (Figure 1) by molecules can be dramatically enhanced by a factor of 10 6 to 10 14 when the molecules are adsorbed onto rough metal surfaces such as Au or Ag or Cu nanoparticles (NPs). [26][27][28] In general, two main mechanisms for Raman enhancement are recognized by researchers. The first mechanism is the most Developing new anticounterfeit technologies with good robustness, high safety index, strong readability, and low cost is highly demanded but challenging. In recent years, anticounterfeiting labels by surface-enhanced Raman spectroscopy (SERS) have drawn great attention due to the molecular encoding, highly accurate identification, large codi...