Abstract: | An assembly of hemispherical Ag nanoparticles is prepared by solid‐state dewetting of thin Ag film deposited on the sapphire substrate. The in situ nanomechanical compression testing of the particles with a flat diamond punch inside the scanning electron microscope demonstrates the deformation behavior typical for the nucleation‐controlled plasticity: high elastic deformation followed by an abrupt particles collapse. The latter is associated with the dislocations nucleation in otherwise pristine particle. The average contact pressure in the contact zone at the onset of dislocation‐controlled plasticity is about 8 GPa, and does not depend on particle size. This observation supports the hypothesis that the pseudoelasticity of much smaller Ag nanoparticles is intrinsically related to their ultrahigh strength. A stress‐induced diffusion along the particle–substrate and particle–punch interfaces is identified as a factor controlling the pseudoelastic deformation. The corresponding diffusion model allows estimating the room‐temperature self‐diffusion coefficient of Ag along the Ag–W and Ag–zirconia interfaces, which is quite close to the estimated value of the grain boundary self‐diffusion coefficient in Ag. Based on this finding, the map of pseudoelastic deformation of crystalline materials is proposed. |