The cold roll bonding process of an Al-Ni layer composite sheet which is applied as a brazing solder for the welding of Nickel and Aluminum structures in the Lithium-ion battery packaging is investigated. The effects of roll bonding and annealing treatment on the application properties and the interface compounds of Al-Ni composite sheet are also studied. The results show that the appropriate rolling reduction to bond and produce Al-Ni layer composite sheet is about 50% to 60% deformation degree. During the annealing process, the first formed Al3Ni phase in the interface of Al and Ni is benefit to the bonding of such two metals but the sequent formed Al3Ni2 phase results in the cracks and separation of the Al-Ni layers. The roll bonding Al-Ni layer composite sheet acquires good bending endurance, stable weldability and suitable electrical resistivity with annealing from 698K to 748K for 1 hour.