Nanoindentation was performed on amorphous silicon nitride films of different thicknesses deposited on gallium arsenide (GaAs) (001) substrates using a conical indenter. Both “pop-in” and ‘pop-out’ were observed from the load-displacement curves when the indentation load exceeded a critical value. Pop-in occurring during loading is associated with plane-slip in the GaAs substrate, and pop-out during unloading is attributed to the interfacial delamination between the film and the substrate. Finite element modeling (FEM) was used to analyze the stress evolution during unloading. The FEM results showed that the stress at the interface evolved from compressive to tensile status during the withdrawal of indentation load, and the interfacial debonding was induced at a critical tensile stress, which is consistent with the pop-out observed. A deformation model for interpreting the pop-in and pop-out events is thereby proposed.