This work reviews the characteristics of layered double hydroxides (LDHs) in the context of protective thin films to enhance the corrosion resistance properties of aluminum alloys. A discussion is made in detail about the LDH protection mechanism and the effect of synthesis approaches on LDH structural variations and the corresponding anti-corrosion behavior. LDHs anion-exchange behavior to host inorganic/organic anions makes them a potential material to investigate for anti-corrosion film. This unique advantage and the availability of a wide range of metal oxide-based layers, interlayer anions, and self-healing properties make LDH family an attractive choice for the development of compact LDHs based smart coating systems.