Abstract: High strength aluminum alloys are used in aerospace industry and are normally coated to prevent corrosion. The corrosion protection of the coatings is mainly provided by pigmented-primer layer. Strontium chromate pigments are widely used, but they are toxic and carcinogenic. The objective of the current study is to develop and characterize the ion exchange compounds bentonite and hydrotalcite as corrosion inhibiting pigments. These compounds were synthesized with different cations and anions, and were used either alone or in mixtures as particulate additive in organic coatings. In coating applications as well as bulk solution, the inhibitor release mechanism is based on ion exchange. To evaluate corrosion inhibition, pigments extract solutions were used in potentiodynamic polarization as well as electrochemical impedance spectroscopy (EIS) experiments on bare aluminum alloy 2024-T3. Cathodic polarization showed that zinc- and cerium-containing filtrate solutions modestly inhibited cathodic current density. These solutions also decreased the extent of pitting damage formed on the surface, as compared to uninhibited 0.5 M NaCl solution. Pigments were also added as primer additives, and painted on AA2024-T3. The coated panels were then subjected to salt spray exposure testing. The possibility of sensing inhibitor exhaustion by means of X-ray diffraction interrogation of the pigment in a coating is demonstrated and discussed on cerium bentonite-pigmented coatings. Although cerium bentonite-pigmented coatings did not show behavior indicative of self-healing, the combination of bentonite and hydrotalcite that released Ce3, Zn2, and PO43− showed potent scribe protection even after 3000 h exposure in salt spray. Promising self-healing was also demonstrated by pigments that consisted of decavanadate-hydrotalcite and zinc pyrovanadate, as indicated by a shiny scribed area after 1000h exposure in salt spray. When these pigments are used, blistering is minimized.