A high-resolution electron microscopy study has uncovered the plastic behavior of accommodating large strains in nanocrystalline (NC) Ni subject to cold rolling at liquid nitrogen temperature. The activation of grain-boundary-mediated-plasticity is evidenced in NC-Ni, including twinning and formation of stacking fault via partial dislocation slips from the grain boundary. The formation and storage of 60? full dislocations are observed inside NC-grains. The grain/twin boundaries act as the barriers of dislocation slips, leading to dislocation pile-up, severe lattice distortion, and formation of sub-grain boundary. The vicinity of grain/twin boundary is where defects preferentially accumulate and likely the favorable place for onset of plastic deformation. The present results indicate the heterogeneous and multiple natures of accommodating plastic strains in NC-grains. A high-resolution electron microscopy study unc uncovered the plastic behavior of accommodating large defects in nanocrystalline (NC) Ni subject to cold rolling at liquid nitrogen temperature. The activation of grain-boundary-mediated-plasticity is evidenced in NC-Ni, including twinning and formation of stacking fault via partial dislocation slips from the grain boundary. The formation and storage of 60? full dislocations are observed inside NC-grains. The grain / twin boundaries act as the barriers of dislocation slips, leading to dislocation pile- up, Severely lattice distortion, and formation of sub-grain boundary. The vicinity of grain / twin boundary is where defects preferentially accumulate and likely the favorable place for onset of plastic deformation. The present results indicate the heterogeneous and multiple natures of accommodating plastic strain in NC -grains.