The influence of rolling on nanomechanical and mechanical behavior of Mg-7Li alloy was investigated by nanoindentation, tensile test and scanning electron microscopy (SEM), respectively. The α-Mg phase elongated along the rolling direction and gradually cracked. As the rolling ratio increased from 3 to 10, the hardness of α-Mg and β-Li phase increased by 7.35% and 20.75%, respectively. The fracture of alloys changed from ductile fracture to quasi-cleavage fracture. The yield strength and ultimate tensile strength increased by 23 MPa and 12 MPa, respectively, while elongation reduced by 12.5%.