Nitrate loss in interflow caused serious nitrate pollution of neighboring water bodies in the purple soil region of China's Sichuan Province. In this study, Mg/Fe(Al)-calcined layered double hydroxides (Mg/Fe(Al)-CLDHs) with varied Mg/Fe(Al) ratios were synthesized for nitrate removal from interflow, and 3:1 Mg/Fe CLDH exhibited the best adsorption performance. The effects of initial pH, adsorbent dosage and co-existing anions on the adsorption performance were investigated by batch experiments. The best-fitting kinetic and isothermal models for nitrate adsorption were the pseudo-second-order model and Freundlich model, respectively, indicating that the adsorption process was a physical-chemical multilayer process. The maximum adsorption capacity of nitrate was 73.36 mg/g, which was higher than that of many other commonly used absorbents. The adsorbents were characterized by XRD, FT-IR, TGA, SEM, TEM and BET techniques, and the XRD and FT-IR results revealed that the adsorption mechanism involved original layered structure reconstruction and ion-exchange interaction. Under the coexistence of SO42− and Cl−, 75.63% nitrate in interflow could be removed after 6 hours of adsorption. Overall, the synthesized Mg/Fe CLDH is an effective and low-cost nitrate absorbent for in-situ nitrate removal.