<p>This study presents a novel framework for analyzing vibration-enhanced degradation to explore atomic-scale bond manipulation in laser-structured superwetting metal surfaces. This framwork integrates a piezoelectric system with multimodal in-situ probing and environmental control. A piezoelectric actuator induces high-frequency oscillations, inducing strain fields that disrupt O-V bonds. Simultaneously, bond strain and adhesion forces are monitored using Raman spectroscopy and atomic force microscopy (AFM). This integrated methodology quantifies the relationship between vibrational parameters, bond stability, and degradation rates, allowing for high-resolution tracking of structural changes under mechanical stress. Moreover, the framework effectively decouples mechanical and chemical degradation pathways, which aids in designing more durable functional surfaces. The findings reveal that vibrational stress significantly accelerates bond reorganization, providing insights into defect-mediated surface evolution and enhancing the understanding of mechanochemical coupling in oxide layers.</p>