Superior structural properties of materials are generally desired in harsh environments, such as elevated temperatures, the high strain rates of impact, and radiation. Composite nanolaminates, built with alternating stacks of metal layers, each with nanoscale individual thickness, are proving to exhibit many of these target properties. In principle, the nanolaminate concept can be applied to any two-phase, bimetallic system; however, they have not been widely applied to materials with a hexagonal close-packed (hcp) crystal structure. Many important structural metals used today belong to the hcp class of materials. Some examples of well-known hcp metals are Mg, Zr, and Ti and their alloys. These alloys are technologically relevant, bearing desirable intrinsic properties, such as low specific density, fatigue resistance, biocompatibility, corrosion resistance, and radiation resistance. Even in coarse-grained traditional form, there is an increasing demand to use hcp materials more often and more broadly in structural applications within the automotive, aircraft, aerospace, biomedical, and nuclear industries. The roadblock to applying the nanolaminate concept to hcp materials is their complex, anisotropic deformation behavior. In this presentation, we discuss recently developed methods to manufacture nanostructured composites containing hcp metals. These techniques exploit plastic deformation as part of the synthesis process and have potential to manufacture product in forms and sizes suitable for high-performance structural applications. One method utilizes severe plastic deformation to make sheets of two-dimensional nanolayered Zr/Nb composite. The material produced exhibits exceptionally high strength and enhanced formability. Another method employs intermediate plastic deformation to create bulk samples of hierarchical three-dimensional nanolayered Zr/Nb composite. The resulting material has a combination of high strength, strain hardening, and ductility. We further highlight in this presentation the modeling and experimental efforts to understand the linkages between the internal nanostructure resulting from processing, local deformation mechanisms, and superior macroscale properties. Although we focus these examples on the Zr/Nb system, the insight gained and manufacturing techniques developed can be applied to other bimetallic systems.