In this work, accumulative pack-roll bonding successfully manufactured the Ni/Ti/Nb multilayer composite. The microstructure evolution and mechanical properties of the composite during the accumulative roll bonding (ARB) process were investigated by scanning electron microscopy (SEM), energy dispersive spectrometer (EDS), transmission electron microscopy (TEM), micro-hardness test, and tensile tests. The results showed that the deformation of each layer was relatively uniform in the initial stage of the ARB process. After the fourth pass, the Ni/Ti interface was still relatively straight, while the Ti/Nb interface was unevenly deformed. After the fourth pass, the microstructure of the Ni layer was equiaxed grains with a decreased grain size of 200 nm, and finer equiaxed grains were observed at the interface. No dynamic recrystallization occurred in the Ti and Nb layers. The laminar structure of the Nb layer was observed, and the grains were oriented parallel to the rolling direction. Moreover, the tensile strength and micro-hardness significantly increased as the number of ARB increased. After five passes of the ARB process, the tensile strength of the composite reached 792.3 MPa, and the micro-hardness of Ni, Ti, and Nb were increased to 270.2, 307.4, and 243.4 HV, respectively.
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