To address the problem of As₄₀Se₆₀ delamination from the sulfur substrate, a simulation model with ZnS, ZnSe, and Ge as the connective layer and As₂Se₃ as the substrate is established using molecular dynamics simulation software. The changes in structural potential energy, total energy, and adsorption energy after vacuum annealing of the simulation model are analyzed. Moreover, ZnS, ZnSe, and Ge monolayer films of the same thickness were prepared in the coating experiments and subjected to the adhesion test. Simulation and experimental results show that ZnS film is prone to shedding, whereas Ge film and ZnSe film do not easily fall off. ZnS film is prone to depacking, but its adhesion to the substrate may be improved by reducing the film thickness and substrate coating temperature.