Two-phase nanolaminate composites have demonstrated an unusually broad number of desirable properties, such as high strength, high strain to failure, thermal stability, and resistance to light-ion radiation. Recently we have shown that nanolaminates with similar exceptional properties can be made via severe plastic deformation (SPD) in bulk sizes suitable for structural applications. While the cause of such attractive properties can easily be associated with a high density of bimetal interfaces, how the interfaces physically control structural properties remains an area of intense research. In this pursuit, we aim to use SPD to fabricate nanolaminates with different types of interfaces. We have found it is possible to change the crystallographic character of the bimaterial interfaces through changes in the SPD processing path. This presentation will highlight our recent modeling and experimental efforts to understand the effects of interfaces on texture evolution, interface character evolution, strength, and plastic anisotropy, during deformation.