Metal corrosion is a persistent industrial issue and contributes to substantial annual economic losses. Advances in anticorrosion technologies are necessary to extend metal substrate lifetimes and prevent losses in performance, especially in marine environments. In this study, a green MXene framework supported with methionine and polyurethane (PU) was synthesized, characterized, and tested as a passive/active anticorrosion technology for a metal alloy substrate. Multiple MAX precursors including Ti3AlC2 were examined using a fluorine-free, nontoxic etching method. Implementing the self-healing properties of PU, reinforcing substrate binding with methionine via hydrogen and disulfide bonding, and maintaining the electrical, electrochemical, and mechanical properties of MXene were the primary objectives of this study. Coating characterization included confirmation of the desired MXene chemical framework and significant thermal stability. The PU self-healing mechanism was demonstrated with a “damaged” MXene/PU coating at room temperature with exposure to UV and visible light. Additionally, anticorrosion testing with artificial seawater yielded high corrosion inhibition efficiency and preserved mechanical properties when exposed to an undamaged and self-healed “damaged” MXene/PU coating.