Abstract: Microrolling experiments and uniaxial tensile tests of pure copper under different annealing conditions were carried out in this paper. The effects of grain size and reduction on non-uniform deformation, edge cracking, and microstructure were studied. The experimental results showed that the side deformation became more non-uniform, resulting in substantial edge bulge, and the uneven spread increased with increasing grain size and reduction level. When the reduction level reached 80% and the grain size was 65 μm, slight edge cracks occurred. When the grain size was 200 μm, the edge cracks became wider and deeper. No edge cracks occurred when the grain size was 200 μm and the reduction level was less than 60%; edge cracks occurred when the reduction level was increased to 80%. As the reduction level increased, the grains were gradually elongated and appeared as a sheet-like structure along the rolling direction; a fine lamellar structure was obtained when the grain size was 20 μm and the reduction level was less than 60%.