As a sensitive analytical measurement, surface enhanced Raman scattering (SERS) technique is gradually attracting the attention of scientists. However, traditional SERS substrate can be easily contaminated and uncomfortably applied into detection in the complex practical samples. In order to enlarge the SERS detection field, in this work, a novel multilayer nanocomposite synthesized by ZnO/GO/Ag is used as SERS substrate. This material can effectively degrade the pollutants absorbed on its surface. Furthermore, the surface of ZnO/GO/Ag is coated by molecular imprinted polymers (MIPs) to synthesize the sandwich SERS imprinted sensor (ZnO/GO/Ag‐MIPs, ZGA‐MIPs), which effectively improves the property of practical sample detection. Through the modern instruments analyzing, the ZGA‐MIPs exhibit satisfying SERS detection properties and selectivity. Importantly, ZGA‐MIPs also possess self‐cleaning property and present favorable recycling capacity. This work provides a novel approach to the SERS detection in the practical samples.