The corrosion inhibition effect of layered double hydroxides (LDHs) and calcined layered double hydroxides (CLDHs) on reinforced concrete under chloride-sulfate attack was studied by approaches of linear polarization resistance (LPR), electrochemical impedance spectroscopy (EIS), energy dispersive spectroscopy (EDS), and chloride ion content test. The results show that CLDHs and LDHs have small particle sizes and large specific surface areas, their micro-aggregate effect can improve the compressive strength of the concrete at 28 d by about 6%, optimize the pore structure of the concrete, and improve the chloride ion binding rate of the concrete system. Under coupled erosion of salt and drying-wetting cycles, CLDHs and LDHs can significantly increase the polarization resistance and capacitive arc of steel bars in reinforced concrete, and the corrosion inhibition efficiency of CLDHs is larger than that of LDHs. With the increase of the number of cycles, the corrosion inhibition efficiency decreases, but the corrosion inhibition efficiency of CLDHs is still above 85% after 90 drying-wetting cycles, and the corrosion inhibition mechanism is mainly originated from the adsorption effect of CLDHs on free chloride ions. Therefore, the addition of CLDHs can effectively improve the corrosion resistance of reinforced concrete.