The absolute grain boundary mobility of 388 nickel grain boundaries was calculated using a synthetic driving force molecular dynamics method; complete results appear in the Supplementary materials. Over 25% of the boundaries, including most of the non-Σ3 highest mobility boundaries, moved by a coupled shear mechanism. The range of non-shearing boundary mobilities is from 40 to 400 m/s GPa, except for Σ3 incoherent twins which have mobilities of 200–2000 m/s GPa. Some boundaries, including all the 〈1 1 1〉 twist boundaries, are immobile within the resolution of the simulation. Boundary mobility is not correlated with scalar parameters such as disorientation angle, Σ value, excess volume or boundary energy. Boundaries less than 15° from each other in five-dimensional crystallographic space tend to have similar mobilities. Some boundaries move via a non-activated motion mechanism, which greatly increases low-temperature mobility. Thermal roughening of grain boundaries is widely observed, with estimated roughening temperatures substantially among boundaries.