The passive film of reinforcing steel in marine concrete is damaged by the infiltration of chloride and sulfate ions. Layered double hydroxide (LDH) can adsorb anions and release interlayer ions to form passive films due to its ion exchange property. A Mg-Al-NO3 layered double hydroxide/montmorillonite (LDH/Mnt) composite inhibitor was prepared by layer-by-layer self-assembly (LBL) of LDH and Mnt. The structure and morphology of the LDH/Mnt composites were characterized by X-ray diffraction (XRD), laser Raman spectroscopy, N2-adsorption/desorption measurements, and transmission electron microscopy (TEM). The LDH/Mnt composites, as inhibitors of chloride ions and sulfate ions, exhibited high slow-release efficiency. The mass ratio of LDH and Mnt affected the curing capacity of the synthesized composites, and the optimum mass ratio was LDH/Mnt = 1:1 for which slow-release efficiency reached 94.16%.