Higher strength and higher ductility are desirable for structural materials. However, ultrastrong alloys inevitably show decreased strain-hardening capacity, limiting their uniform elongation. We present a supranano (<10 nanometers) and short-range ordering design for grain interiors and grain boundary regions, respectively, in fine-grained alloys based on vanadium, cobalt, and nickel, with additions of tungsten, copper, aluminum, and boron. The pronounced grain boundary-related strengthening and ductilization mechanism is realized through segregation of the short-range ordering near the grain boundary. Furthermore, the supranano ordering with a larger size has an enhanced pinning effect for dislocations and stacking faults, multiplied and accumulated in grain interiors during plastic deformation. These mechanisms promote continuously increased flow stress until fracture of the alloy at 10% strain with 2.6-gigapascal tensile stress.