In this work, we consider the physical basis of deformation and fracture in layered composite nanocrystalline/amorphous material–low-melting crystalline alloy in a wide temperature range. Deformation and fracture at the crack tip on the boundary of such materials as nanocrystalline alloy of the trademark 5BDSR, amorphous alloy of the trademark 82K3XSR and low-melting crystalline alloy were experimentally investigated. The crack was initiated by uniaxial stretching in a temperature range of 77–293 K. A theoretical description of the processes of deformation and fracture at the crack tip is proposed, with the assumption that these processes lead to local heating and ensure the plastic character of crack growth at liquid nitrogen temperatures. The obtained results improve the theoretical understanding of the physics of fracture at the boundary of nanocrystalline and crystalline alloys in a wide temperature range. The possibility of preserving the plastic nature of fracture in a thin boundary layer of crystalline–nanocrystalline material at cryogenic temperatures has been experimentally shown.