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MXenes with unique physicochemical properties have shown substantial potential in electromagnetic interference (EMI) shielding. However, the chemical instability and mechanical fragility of MXenes has become a major hurdle for their application. Abundant strategies have been dedicated to improving the oxidation stability of colloidal solution or mechanical properties of films, which always come at the expense of electrical conductivity and chemical compatibility. Here, hydrogen bond (H‐bond) and coordination bond are employed to achieve chemical and colloidal stability of MXenes (0.1 mg mL−1) by occupying the reaction sites of Ti3C2Tx attacking of water and oxygen molecules. Compared to the Ti3C2Tx, the Ti3C2Tx modified with alanine via H‐bond shows significantly improved oxidation stability (at room temperature over 35 days), while the Ti3C2Tx modified with cysteine by synergy of H‐bond and coordination bond can be maintained even after 120 days. Simulation and experimental results verify the formation of H‐bond and Ti‐S bond by a Lewis acid‐base interaction between Ti3C2Tx and cysteine. Furthermore, the synergy strategy significantly improves the mechanical strength of the assembled film (up to 78.1 ± 7.9 MPa), corresponding the increment of 203% compared to untreated one, almost without compromising the electrical conductivity and EMI shielding performance.

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