The initial excitation of interface crack of large-size ultra-thin chips is one of the most complicated technical challenges. To address this issue, the reversible fracture characteristics of a silicon-based chip (chip size: 1.025 mm × 0.4 mm × 0.15 mm) adhesive layer interface was examined by scanning electron microscope (SEM) tests, and the characteristics of a cohesive zone model (CZM) unit were obtained through peel testing. The fitting curve of the elastic bilinear model was in high agreement with the experimental data, with a correlation coefficient of 0.98. The maximum energy release rate required for stripping was GC = 10.3567 N/m. Subsequently, a cohesive mechanical model of large-size ultra-thin chip peeling was established, and the mechanical characteristics of crack initial excitation were analyzed. The findings revealed that the larger deflection peeling angle in the peeling process resulted in a smaller peeling force and energy release rate (ERR), which made the initial crack formation difficult. To mitigate this, a coupling control method of structure and force surface was proposed. In this method, through structural coupling, the change in chip deflection was greatly reduced through the surface coupling force, and the peeling angle was greatly improved. It changed the local stiffness of the laminated structure, made the action point of fracture force migrate from the center of the chip to near the edge of the chip, the peeling angle was increased, and the energy release rate was locally improved. Finally, combined with mechanical analysis and numerical simulation of the peeling process, the mechanical characteristics of peeling were analyzed in detail. The results indicated that during the initial crack germination process, the ERR of the peel interface is significantly increased, the maximum stress value borne by the chip is significantly reduced, and the peel safety and reliability are greatly improved.