Abstract Grain refinement can drastically increase the strength of metals. However, this approach tends to become less effective or even inverses once grain sizes are reduced to very small scales, generally below 10 ~ 20 nanometers. This softening effect emerges from grain boundary instability and the limited ability of dislocations to form and move within such nanosized grains. However, grain boundary stability can be tuned by solute decoration or grain boundary relaxation.