The flawless nanocrystalline (nc) Ni with a broad grain size distribution ranging from 5 to 120 nm and an average grain size of 20-30 nm were prepared by direct current and pulse electrodeposition, respectively. In the region of room-temperature static tensile strain rates, for the nc Ni prepared by direct current electrodeposition, the average ultimate tensile strength and the average elongation to failure are 1176 MPa and 10.6%, respectively. While for the nc Ni prepared by pulse electrodeposition, the ultimate tensile strength exceeds 1500 MPa and the max elongation to failure reaches 13.3%. In contrast to the typical electrodeposited nc Ni with a narrow grain size distribution below 50 nm, the ductility is increased by more than 100% for the present nc Ni samples. This enhancement can be interpreted by the reason that dislocations can exist and multiply in the large grains by the mechanism of Frank-Read source in the plastic deformation process revealed by theoretical calculation.