A theoretical model is suggested which describes cooperative action of grain boundary (GB) sliding and rotational deformation in mechanically loaded nanocrystalline materials. Focuses are placed on the crossover from GB sliding to rotational deformation occurring at triple junctions of GBs. In the framework of the model, gliding GB dislocations at triple junctions of GBs split into dislocations that climb along the adjacent boundaries. The splitting processes repeatedly occurring at triple junctions give rise to climb of GB dislocation walls that carry rotational deformation accompanied by crystal lattice rotation in grains of nanocrystalline materials. The role of GB sliding, rotational deformation and conventional dislocation slip in high-strain-rate superplastic flow in nanocrystalline materials is discussed.