Introduction: Semiconductor-based surface-enhanced Raman scattering (SERS) substrates with high stability and reproducibility have become one of the essential analytical tools in the analysis of chemical and biological at trace levels. Herein, a growth of the hexagonal-wrapped ZnO nanorod arrays decorating with Ag nanoparticles (AgNPs) at different concentrations of Ag was proposed. Methods: The crystallinity, morphology, chemical composition, and optical properties of the prepared samples were investigated by X-ray powder diffraction (XRD) and field emission scanning electron microscopy (FE-SEM), energy-dispersive X-ray spectroscopy (EDX), Raman system, respectively. Results: The results revealed that the SERS performance of ZnO NRs incorporating with AgNPs exhibited higher detection of crystal violet (CV) probe molecules at a low concentration of 10􀀀8 M than that of the pristine ZnO NRs. This effect originates from the localized surface plasmonic resonance of AgNPs that could cause a strong electromagnetic field and synergistic effects of Ag, ZnO, and CV molecules in ZnONRs@Ag/CV SERS system. Conclusion: These outcomes reveal that AgNPs play a crucial role in enhanced SERS performance for chemical and biological detection of ZnO substrate.