Ultrafine-grained pure metals and their alloys have high strength and low ductility. In this study, cryorolling under different strains followed by low-temperature short-time annealing was used to fabricate pure nickel sheets combining high strength with good ductility. The results show that, for different cryorolling strains, the uniform elongation was greatly increased without sacrificing the strength after annealing. A yield strength of 607 MPa and a uniform elongation of 11.7% were obtained after annealing at a small cryorolling strain (ε = 0.22), while annealing at a large cryorolling strain (ε = 1.6) resulted in a yield strength of 990 MPa and a uniform elongation of 6.4%. X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM), and electron backscattered diffraction (EBSD) were used to characterize the microstructure of the specimens and showed that the high strength could be attributed to strain hardening during cryorolling, with an additional contribution from grain refinement and the formation of dislocation walls. The high ductility could be attributed to annealing twins and micro-shear bands during stretching, which improved the strain hardening capacity. The results show that the synergistic effect of strength and ductility can be regulated through lowtemperature short-time annealing with different cryorolling strains, which provides a new reference for the design of future thermo-mechanical processes.