Surface-enhanced Raman scattering (SERS) enables pesticide residue monitoring to become facile and efficient. In this study, a core-shell structured gold nanoparticles@ZnCo metal-organic framework (AuNPs@ZnCo-MOF) SERS substrate was designed and successfully synthesized for efficient and selective detection of thiram. The bimetallic ZnCo-MOF shell can not only enrich the targeted molecules in the electromagnetic field because of its excellent absorptive capacity, but also act as a stabilized matrix for protecting the AuNPs from aggregation. The AuNPs@ZnCo-MOFs exhibited a high enhancement factor (EF) of 3.51 × 10