This study demonstrates an approach of utilizing high-pressure torsion (HPT) to fabricate a novel hybrid material by the direct bonding of Al and Ti disks at room temperature under a compressive pressure of 6.0 GPa and with increasing numbers of HPT turns up to 50. Detailed structural observations revealed the formation of a multi-layered nanostructure in the edge regions of the disks with a grain size of ∼30 nm. X-ray diffraction (XRD) and selected area electron diffraction (SAED) confirmed the presence of three intermetallic compounds, AlTi, Al3Ti and Ti3Al, in the layered structures. Processing by HPT led to the formation of a hybrid nanocomposite with exceptional hardness (over 300 Hv) in the edge regions of the disks. Special emphasis was placed on understanding the evolution of hardness in the hybrid material. The investigation demonstrates a significant opportunity for using HPT processing to deepen the knowledge on diffusion bonding and mechanical joining technologies as well as for fabricating new and valuable hybrid nanomaterials.