AA1050/AA5052 multilayer laminate sheets were fabricated by accumulative roll bonding (ARB) and cryorolling (CR). The ultimate tensile strength (UTS) of the laminate sheets produced by combining ARB and CR increased up to 18.4% compared to that by five ARB passes. Necking and fracture occurred in the hard layer after the fourth ARB pass. In contrast, the hard layer remained continuous and relatively straight during CR, which suggested that CR can delay the onset of necking and fracture. TEM results showed that CR can not only refine grain size but also significantly improve interfacial bonding quality. CR can accumulate higher dislocation density. Therefore, the laminate sheets prepared by the combination of ARB and CR obtained better mechanical properties than that by five ARB passes.