Self-healing polyurethane (PU) faces aging deterioration due to active dynamic bonds, which remain a challenging predicament for practical use. In this work, a novel strategy is developed to address this predicament by leveraging the hydrophobicity and gas barrier of hydrogenated hydroxyl-terminated polybutadiene (HHPB). The dynamic oxime-carbamate bonds derived from 2, 4-pentanedione dioxime (PDO) enable the elastomer to exhibit surface self-repairability upon applied mild heat and achieve similar to 99.5% mechanical self-healing efficiency. The mechanical properties remained nearly intact after 30-d exposure to thermal oxidation, xenon lamp, acids, bases, and salts. Gas permeability, positron annihilation lifetime spectroscopy (PALS), and contact angle measurements reveal the pivotal role of gas barrier, free volume, and hydrophobicity in blocking undesirable molecules and ions which effectively protects the elastomer from deterioration. HHPB-PU also exhibits excellent adhesion to steel substrate. The shear strength achieves (3.02 +/- 0.42) MPa after heating at 80 degrees C for 4 h, and (3.06 +/- 0.2) MPa after heating at 130 degrees C for 0.5 h. Regarding its outstanding anti-corrosive and weatherproof performances, this self-healable elastomer is a promising candidate in surface-protective applications.
