The constant challenge of corrosion significantly compromises the durability and functionality of metal substrates, propelling the demand for advanced protective solutions. This study introduces a novel smart epoxy coating system modified with a three-component nanocomposite integrating polydopamine (PDA)-modified Ti3C2 MXene with ZnAl-layered double hydroxides (LDH), intercalated with phosphate (P) and glutamate (Gl) ions as corrosion inhibitors. The innovative approach leverages the synergistic impacts of barrier protection, ion exchangeability, and self-healing capabilities to offer superior anti-corrosion performance. In the solution phase, the EIS results revealed a notable increase in resistance values, with MPLG samples exhibiting a 2.45-fold and MPLP samples a 2.17-fold enhancement compared to the blank specimen after 96 h of immersion. Furthermore, the data obtained from EIS demonstrated a significant enhancement in the barrier effects of the epoxy coating upon the addition of MPLG and MPLP. This enhancement was evidenced by a significant increase in the impedance values, which were observed to be 103-fold higher following a prolonged immersion period of 140 days. The self-healing properties, confirmed through EIS, FE-SEM, and EDX/Mapping analyses, indicated the formation of a stable corrosion-protective layer over the damaged areas, thus providing active protection. Adhesion assessments further underscored the coatings' durability, with MPLG and MPLP samples demonstrating minimal delamination. Collectively, these findings emphasize the potential of the proposed PDA-modified MXene@ZnAl-LDH nanocomposite as a multifaceted solution to corrosion challenges, promising significant advancements in the longevity and reliability of coated metal surfaces.