Nanocrystalline (NC) metals have attracted widespread interest in materials science due to their high strength compared to coarse-grained counterparts. It is well know that during uniaxial deformation, the stress-strain behaviour exhibits an extraordinary work-hardening followed by an early observation of constant flow stress. Information on possible deformation mechanisms have been gathered by extensive research combining in situ deformation experiments, electron microscopy observations and computational modelling. Generally, these mechanisms are categorized into two types: dislocation slip and grain boundary (GB) accommodation processes, as for instance, GB sliding based mechanisms and GB migration eventually coupled to the shear stress. However, the interplay between these mechanisms resulting in the constant deformation resistance is not fully understood. Transient testing has proven to be a suitable tool to gather information on the rate limiting deformation mechanisms that are activated during the deformation path. In particular in stress reduction experiments, after an intermediate/large stress drop thermally activated dislocation slip is suppressed so that other underlying mechanisms are brought into foreground during subsequent transient creep. Those mechanisms may play a minor role in the determination of the flow stress but might still be essential to the development of a constant deformation resistance. Within this thesis, transient testing is combined with in situ X-ray diffraction at the Swiss Light Source. Therefore, the transient responses are captured in terms of evolution of macrostrain as well as diffraction peak broadening. Since dislocation slip and GB accommodation have an opposite footprint on the peak broadening, the presence of these two types of mechanisms can be distinguished. Three electrodeposited NC materials with different grain sizes are investigated: two NC Ni batches and one NC Ni50Fe50 batch. The results reveal that the constant flow stress reached during uniaxial deformation of electrodeposited NC metals reflects a quasi-stationary balance between dislocation-based mechanisms and GB-mediated accommodation. The latter plays an important role in producing plastic strain and recovering the defects and internal stress. Depending on the magnitude of the stress drop, a non-monotonic behaviour of the diffraction peak width is observed, suggesting an alternation of mechanisms. Also, by comparing transient responses among different NC materials, the relative contributions of dislocation slip and GB accommodation mechanisms are discussed in terms of grain size and alloying. Finally, different magnitudes of stress reduction are carried out by molecular dynamics (MD) simulations with the aim to verify in situ experimental results and explore the mechanisms responsible for GB accommodation. MD simulations confirm that dislocation slip is reduced after a moderate stress drop, however can continue to operate after adaption of the GB structures by a variety of GB accommodation mechanisms explaining the non-monotonic behaviour of the peak broadening during transient creep.