Grain boundary affects the microstructure of metal material, and thus further its macroscopic properties. As is well known, under the action of applied stress, the grain boundary migrates. The structures and arrangements of grain boundary dislocations at different misorientation angles are very different, which affects the macrophysical and chemical properties of metal crystal. Therefore, it is of great theoretical and practical significance to study the dislocation structure and reaction mechanism of grain boundary under different misorientations for further studying the material properties.The phase field crystal method is used to simulate the low-angle asymmetric tilt grain boundary structure and dislocation motion on a nanoscale. From the perspective of the change of the position of the grain boundary dislocation motion under the applied stress and the change of the free energy of the crystal system, the influences of the misorientation angle on the low-angle asymmetric tilt grain boundary structure and the motion of the grain boundary dislocation are analyzed. The results show that the types of dislocation pairs of low-angle asymmetric tilt grain boundaries at different misorientation angles are the same. With the increase of misorientation angle, the grain boundary dislocation pairs increase, and n1n2 and n4n5 type dislocation pairs are more easily formed at the grain boundaries. Under the action of applied stress, the initial movement states of the grain boundary dislocation pairs at different misorientation angles are all climbing along the grain boundaries. As the system energy accumulates, the larger the misorientation angle is, the more the number of decomposed grain boundary dislocation pairs decomposed will be, and only in the dislocation pairs of n1n2 and n4n5 type there occurs decomposition reaction. There are four stages in the free energy curve of the low-angle asymmetric tilt grain boundary system at different misorientation angles, which correspond to the dislocation pairs climbing, dislocation pairs sliding and decomposition, dislocation pairs reaction to form single crystal, and the free energy rising process of the system. Further research shows that as the misorientation angle increases, the time for the single crystal system formed by the dislocation of grain boundary pairs to annihilate is required to be long.