A multi-metal composite was consolidated from the Ti50Ni25Cu25and Fe50Ni33B17alloys by room-temperature high-pressure torsion (HPT). The structural research methods used in this study were X-ray diffractometry, high-resolution transmission electron microscopy, scanning electron microscopy with an electron microprobe analyzer in the mode of backscattered electrons, and the measurement of indentation hardness and modulus of the composite constituents. The structural aspects of the bonding process have been examined. The method of joining materials using their coupled severe plastic deformation has been established to play a leading role in the consolidation of the dissimilar layers upon HPT.