Over the past 3-5 years, the ability to process interface dominant nanolayered bimetallic composites in bulk quantities has opened new opportunities for investigations into structural material behavior under extreme strains. This article reviews the emergence of mechanically stable, predominant bimetallic interface characters during nanomaterial synthesis via Accumulative Roll Bonding, a severe plastic deformation technique. This processing method itself imposes an extreme condition. We show that the interfaces that are naturally selected by this extreme operation remarkably prove to be stable under exposure to other extreme conditions, including elevated temperatures and ion irradiation. Through control of synthesis pathways, interfaces of the desired atomic structure can be manufactured using scalable thermomechanical processing techniques. This, in turn, opens unprecedented new possibilities for designing bulk materials with interface-dominant properties including enhanced strength, deformability, thermal stability, and radiation damage tolerance.