Here, we develop a new method to improve the surface enhanced Raman spectroscopy (SERS) activity of ZnO using Mg doping combined with noble metals. Highly aligned silver nanoparticles (AgNPs) decorated on an array of Mg-doped ZnO (MZOgAg) were fabricated. Using rhodamine 6G as the probe molecule, SERS indicated that the MZO@Ag substrate possesses perfect sensitivity, homogeneity, and chemical stability. The enhancement mechanism of this substrate was analyzed in detail, and finite-difference time-domain (FDTD) simulations were used to examine "hot spot" distribution which generated gaps between the balls, the rods, and the stems. FDTD simulation calculated (E/E-0)(4) to be 2.5 X 10(6). Furthermore, the prepared substrates could degrade the target molecules in situ irradiated by visible light irradiation over the course of 40 min and then efficiently recover detectability through a recycling process. Our substrates were easy to fabricate, self-cleaning, and reusable. They are expected to provide new opportunities for the use of SERS in biological sensors, biomedical diagnostics, and food safety.