Laminate sheets attract increasing attention from researchers and engineers. In this paper, Al/Ti/Al laminate sheets were fabricated by using cryogenic roll bonding for first time. The edge defects, mechanical properties, and interface bonding of laminate sheets by cryogenic roll bonding technique were compared with these by room-temperature roll bonding technique. Results show that there are some edge cracks in laminate sheets by room-temperature roll bonding while they do not appear when subjected to cryogenic roll bonding. The ultimate tensile stress of laminate sheets by cryogenic roll bonding increases up to 36.7% compared to that by room-temperature roll bonding. When laminate sheets are rolled to 0.125 mm from 2.025 mm, the interfaces between Al and Ti layers are bonded well for both cryogenic roll bonding and room-temperature roll bonding. Finally, we discussed the improvement in edge quality and mechanical properties and the mechanism of interface bonding of Al/Ti/Al laminate sheets during cryogenic roll bonding.