Heavy plastic deformation may refine grains of metals and make them very strong. But the strain-induced refinement saturates at large strains, forming three-dimensional ultrafine-grained (3D UFG) structures with random orientations. Further refinement of this microstructure is limited because of the enhanced mobility of grain boundaries. Very-high-rate shear deformation with high strain gradients was applied in the top surface layer of bulk nickel, where a 2D nanometer-scale laminated structure was induced. The strongly textured nanotaminated structure (average lamellar thickness of 20 nanometers) with low-angle boundaries among the lamellae is ultrahard and ultrastable: It exhibits a hardness of 6.4 gigapascal—which is higher than any reported hardness of the UFG nickel—and a coarsening temperature of 40 kelvin above that in UFG nickel