Surface impregnation of concrete structures with a migrating corrosion inhibitor is a promising and non-invasive technique for increasing the lifetime of existing structures that already show signs of corrosion attack. The main requirement for inhibitors is their ability to diffuse the rebar at a sufficient rate to protect steel. The use of smart nanocontainers such as layered double hydroxides (LDH) to store corrosion inhibitors significantly increases efficiency by providing an active protection from chloride-induced corrosion. The addition of LDH to reinforced mortar can also improve the compactness and mechanical properties of this matrix. Here, we report the synthesis of a magnesium–aluminum LDH storing glutamine amino acid as a green inhibitor (labeled as Mg–Al–Gln), which can be used as a migrating inhibitor on mortar specimens. The corrosion behavior of the specimens was determined via electrochemical techniques based on measurements of corrosion potential and electrochemical impedance spectroscopy. A cell containing a 3.5% NaCl solution was applied to the mortar surface to promote the corrosion of embedded rebars. The specimens treated with Mg–Al–Gln presented an improved corrosion protection performance, exhibiting an increase in polarization resistance (Rp) compared to the reference specimens without an inhibitor (NO INH). This effect is a consequence of a double mechanism of protection/stimuli-responsive release of glutamine and the removal of corrosive chloride species from the medium.