The deformation behavior of nanocrystalline Ni–W alloys is evaluated by nanoindentation techniques for grain sizes of 3–150nm, spanning both the range of classical Hall–Petch behavior as well as the regime where deviations from the Hall–Petch trend are observed. The breakdown in strength scaling, observed at a grain size of 10–20nm, is accompanied by a marked transition to inhomogeneous, glass-like flow (i.e. shear banding) at the finest grain sizes approaching the amorphous limit. As a consequence of this mechanistic crossover, additional inflections arise in the mechanical properties; maxima are observed in both the rate and pressure dependence of deformation at approximately the same grain size as the onset of the Hall–Petch breakdown. These data experimentally connect the mechanical properties of nanocrystalline alloys to the well-known behavior of amorphous metals.