The doping of Al & sum;5(210) grain boundaries with eight different solute atoms was simulated using molecular dynamics, and the effects of different doping elements, temperatures, and doping contents on the energies, microstructures of grain boundaries, and dislocations were investigated. The results show that the doping of Ti, V, and Zr elements can effectively reduce the grain boundary energy of the Al & sum;5(210) grain boundaries, and the higher the doping content, the greater the effect on the grain boundary energy, while the Cu and Ti elements have a good ability to segregation in Al & sum;5[001](210) grain boundaries. With the increase of temperature, the dislocations gradually undergo annihilation, and the dislocations in the Al & sum;5(210) grain boundaries are most affected at 900 K. The dislocations in the Al & sum;5[001](210) grain boundaries are well affected by the increase of temperature. With the increase of solute atom content, a significant lattice distortion is produced, which makes the grain boundary structure of & sum;5(210) more affected.