Ultra-large compressive plasticity at room temperature has recently been observed in electrodeposited nanocrystalline nickel (nc-Ni) under micro-scale compression (Pan, Kuwano, Fujita and Chen: Nano Lett. Vol. 7 (2007), p. 2108). With aid of a TEM sample preparation technique employing focused ion beam (FIB), TEM observations on deformed nc-Ni evidenced deformation-induced microstructural evolution of nc-Ni at a variety of strain levels: Whilst the deformation increases, substantial grain growth is uncovered in the nc-Ni. No apparent ex situ evidence of intragranular dislocation activities is found in the deformed sample. As thermal diffusion plays an insignificant role in the deformation in nc-Ni at room temperature (∼0.17Tm), this premium plasticity is achieved in accommodation with the grain-boundary-mediated deformation, with assistance of extensive grain growth that is mainly driven by high stresses at steady plastic flow.