Due to the current unhealthy diet structure and lifestyle habits, as well as the aging population and other factors, the incidence of chronic diseases such as hypertension is gradually increasing, and people gradually favor antihypertensive health food. However, in order to improve the efficacy of healthy food, there are unscrupulous businessmen in the market who illegally add antihypertensive drugs, especially sartans antihypertensive drugs, to healthy food. Based on the above phenomenon, this study established a Thin-Layer Chromatography (TLC) and Surface-enhanced Raman spectroscopy (SERS) method to investigate five possible prohibited ingredients of sartans (Olmesartan Medoxomil, Irbesartan, Losartan potassium, Telmisartan and Valsartan) in antihypertensive health food products. In this study, we investigated the optimal conditions for the SERS detection of five drugs, compared the effects of TLC spreaders with different ratios of different components on the separation of the five drugs. We successfully obtained the separation system of cyclohexane-ethyl acetate-methanol-glacial acetic acid=53∶35∶12∶0. 25 (v/v/v/v) after extensive formulation tests. After determining the exact conditions of this experiment, the preliminary separation of drug standard solution, mock positive sample solution and real sample solution was carried out by using TLC separation technique. After separation, gold gel was added dropwise at the spot in situ with different ratio shift values on the thin layer plate for SERS detection. The SERS spectra of drug standard solution as well as mock positive sample solution at the spot in situ were collected, compared and determined. The results showed that the five prohibited additive ingredients of sartans could be clearly separated by TLC, their SERS spectra were consistent and reproducible, and the qualitative analysis could be performed quickly according to their respective characteristic peaks, with detection limits between 0. 1 and 1 mg·kg-1. The TLC-SERS method established in this study is simple and rapid. It can provide a reference for the simultaneous on-site rapid detection of prohibited added ingredients in health food.