 The emerging gradient nanostructured metals and alloys containing spatially graded structural components with large variations in length scale and or mechanical properties exhibit unprecedented mechanical performance. This perspective delineates the basic structural features of gradient nanostructures, structural components and spatial gradients, as well as related synthesis methods, excellent tensile properties, and novel deformation mechanisms. The challenges and prospect for the development of gradient nanostructured materials in the future are also addressed. This article was authored by Pantingsong and Lulay.