<div>Atomistic simulations are used in this project to study the deformation mechanism of polycrystalline and bicrystal of pure Al and Al-Mg alloys. Voronoi Tessellation was used to create three-dimensional polycrystalline models. Monte Carlo and Molecular</div><div>Dynamics simulations were used to achieve both mechanical and chemical equilibrium in all models. The first part of the results showed improved strength, which is included the yield strength and ultimate strength in the applied tensile loading through the addition of 5 at% Mg to nanocrystalline aluminum. By viewing atomic structures, it clearly shows the multiple strengthening mechanisms related to doping in Al-Mg alloys. The strength mechanism of dopants exhibits as dopant pinning grain boundary (GB) migration at the early deformation stage. At the late stage where it is close to the failure of nanocrystalline materials, Mg dopants can stop the initiation of intergranular cracks and also do not let propagation of existing cracks along the GBs. Therefore, the flow stress will improve in Al-Mg alloy compared to pure Al. In the second part of our results, in different bicrystal Al model, Σ 3 model has higher strength than other models. This result indicates that GB structure can affect the strength of the material. When the Mg dopants were added to the Al material, the strength of sigma 5 bicrystal models was improved in the applied shear loading. </div><div><br></div><div>However, it did not happen for Σ 3 model, which shows Mg dopants cannot affect the behavior of this GB significantly. Analysis of GB movements shows that Mg dopants stopped GBs from moving in the Σ 5 models. However, in sigma 3 GBs, displacement of grain boundary planes was not affected by Mg dopants. Therefore, the strength and flow stress are improved by Mg dopants in Σ 5 Al GBs, not in the Σ 3 GB.</div>