Laser debonding technology has been widely used in advanced packaging of high-performance chips, such as chiplet, high bandwidth memofy, fan-out, and 2.5/3-dimensional and other packages. However, there are few reports on how the domain-limiting effect in wafer stacking structures affects the laser stripping difficulty and ablation threshold of organic bonding materials. Here, we propose a new method to reduce the laser debonding threshold of temporary bonding materials (TBM) based on the enhancement of the domain-limiting effect. Compared with the surface ablate approach, the domain-limited confinement effect is able to gather the laser-induced plasma in the confined-domain space to produce higher transient temperatures as well as durations, which reduces the ablation threshold of the TBM. The increase in modulus of the TBM layer enables the enhancement of the domain-limiting effect, which facilitates the extension of laser-induced shocks in the horizontal plane. The optimized high-modulus monolayer TBM can be debonded without damage during laser beam scanning at low energy density (150 mJ/cm). It provides sufficient theoretical support for the development of next-generation, large-sized, ultrathin wafer-level debonding in the field of advanced packages.