The laminated metal composites (LMCs) of dissimilar metals (aluminium alloys: AA1100/AA7075) were fabricated using the accumulative roll bonding technique in conjunction with cold rolling. The LMCs of ultrafine grained AA1100 and nanostructured precipitates of AA7075 achieved metallurgical bonding. The microstructure of the bonding interfaces and constituent metals was investigated using scanning electron microscopy and transmission electron microscopy for the LMCs with different layers. The deformation incompatibility and shear actions were analyzed using the microanalysis of dissimilar bonding interfaces. The mechanism of grain refinement of LMCs was investigated and described based on the microstructure characterization. The mechanical properties, strengthening mechanism, and fracture mechanism of LMCs were also investigated. The research results showed that the strengthening mechanism of LMCs is the recombination action of grain refinement, dislocation, and laminated interfacial strengthening. The coordinated deformation of dissimilar metals and the layer thickness are important in improving the mechanical properties of LMCs consisting of dissimilar metals.