The combination of interlocked lamellae grains is the primary feature of biological material “nacre” to constitute its highest strength. The mimic of this hierarchical assembly of biological material combinations remains the challenge for the future trending bioinspired engineering materials. In this study, the interlocked nanolaminated architecture of graphene-reinforced aluminum alloy nanocomposite achieved via multi-step powder metallurgy route and industrial extrusion process followed by laser shock peening. Interrupted re-nucleation to obtain lamellae grains, controlled laminates sliding through interlock mechanism and inhibited large dislocation loop formation in the nanocomposites during laser shock peening was significantly influenced the mechanical properties of the nanocomposites. Consequently, enhancement in the hardness, tensile strength, wettability characteristic properties and prolonged fatigue life cycles were achieved significantly for nanocomposites.