It is possible to produce a nanocrystalline, multilayered composite structure with enhanced mechanical properties by assembling three 316L surface nanostructured stainless steel plates by roll bonding. The Surface Mechanical Attrition Treatment (SMAT) was first used to generate nanocrystalline layers on the elementary plates so that their mechanical properties were improved. They were then assembled through co-rolling. A composite structure of nanocrystalline layers of high strength alternating with more ductile layers was obtained to achieve both high strength and ductility. Microscopy observations and EBSD measurements were carried out and the bonding interfaces were analysed in detail to explore the mechanisms involved during the SMAT/Co-rolling duplex process.