The modified CaAl-LDHs corrosion inhibitor (CaAl-EDTA LDH) was prepared by calcination reduction method with EDTA-2Na as modifier, and the effect of CaAl-EDTA LDH on the macro-properties (fluidity, setting time, mechanical properties) and micro-properties (product composition, hydration heat, pore structure) of cement-based materials was investigated. Besides, two corrosion modes were set up to simulate the protective effect of CaAl-EDTA LDH with different content (0%, 0.5%, 1.0%, 2.0%, 4.0%, mass fraction) on the embedded reinforced mortar specimens. The results show that the addition of 0.5% and 1.0% CaAl-EDTA LDH promotes the dissolution of cement minerals, increases the hydration heat release, and improves the early strength of mortar. However, EDTA has a retarding effect. When the content of CaAl-EDTA LDH is 4.0%, the hydration heat release and the formation of early hydration products of mortar seriously reduces, while the paste total porosity of 28 d increases by about 4%. Moreover, corrosion test results indicate that CaAl-EDTA LDH does not show corrosion resistance in dry-wet cycle mode, while it shows excellent corrosion resistance on reinforcement in mortar after 90 times dry-wet cycle under dual corrosion mode with the content controlled in 1.0%~2.0%. The new type of corrosion inhibitor in this paper has reference significance for prolonging service life of reinforced concrete and improving durability of structures.