Carbendazim (Methyl-1H-2-benzimidazole carbamate),a kind of broad-spectrum fungicide, is extensively used in the prevention and treatment of ring rot and brown spot in apple planting. However, excessive use and residue of Carbendazim induce toxic effects on humans.In order to rapidly and accurately detect Carbendazim in apples, the Surface-Enhance Raman Spectroscopy combined immunoassay (SERSIA) was used in this study. This method was based on SERS’s highly sensitive molecular “fingerprint” characteristics, combined with immunospecific selectivity. The core-molecule-shell “sandwich” structure of Au@M@Ag nano SERS material and SERS immune probe binding antigen were prepared. Combined with Fe3O4 magnetic nanomaterial coated antibody,the specific detection of Carbendazim was achieved with the separable function.Transmission electron microscopy (TEM), UV-Vis spectroscopy and Raman spectroscopy were used to characterize the material properties and optimize the experimental parameters.The results showed a good linear relationship between 0.5～300 nmol·L-1 carbendazim concentration and the intensity of Characteristic peak at 2 227 cm-1 of the labeled molecule 4-mercaptobenzonitrile. The average recovery of Carbendazim in apples with different spiked concentrations was 95.6%～98.3%, and the RSD value was 0.15%～0.99%. Itis a sensitive, selective and stable method for detecting Carbendazim in apples without complex pretreatment.