The surface strengthening agents OTR202 and OTR103 are used as active substrate of the surface enhanced Raman spectroscopy (SERS), and the rapid detection method of the carbaryl solution based on SERS is explored in this research. Firstly, the contrastive analysis of the normal Raman and SERS spectra of the carbaryl solution is proposed. Secondly, the effect of the surface strengthening agents and the addition amount of the measured samples on SERS spectra of the carbaryl solution is investigated. Lastly, SERS spectra of the carbaryl solution in the concentration range of 0.1~15.0 mg/L are analyzed. The linear regression is made between the intensity of characteristic peaks at 1374 cm-1 and the concentration of the carbaryl solution, the linear regression equation is y=414.5x + 481.59, and the determination coefficient R2 is 0.9864. The experimental results show that the detection limit for the carbaryl solution is 0.1 mg/L, and the detection method, which is applied in the surface strengthening agents OTR202 and OTR103 as active substrate, can be used to detect the carbaryl residue in water.