We conducted in situ microtension experiments in a scanning electron microscope (SEM) to study the orientation-dependent mechanical behavior of nanolaminated graphene-Al composite. We found a transition from a weak-and-brittle behavior in the isostress composite configuration to a strong-yet-ductile tensile response in the composite under isostrain condition. This is explained by the excellent load-bearing capacity of the graphene nanosheets and a crack deflection mechanism rendered by the laminate structure. These in situ measurements enabled direct observation of the deformation procedure and the exact failure mode, which highlight the importance of microstructural control in tailoring the mechanical properties of advanced metal matrix composites (MMCs).