This communication describes a new surface-enhanced Raman scattering (SERS) active silver substrate prepared by iodination of the evaporated silver foil. After iodination, the morphology of the silver substrate undergoes a self-evolution process in which it displays accordingly the UV-vis absorption shift as well as the AFM topological test. Rhodamine 6G (R6G) is used as the probe molecule to evaluate the enhancement efficiency of the silver substrate at different self-evolution time intervals. The SERS intensity of R6G increases up to ∼29-fold and reaches a maximum after the substrate evolved for 24 h. This method is feasible for the production of an efficient SERS silver substrate.