We have examined the interplay between magnetism and dislocation core properties in NiAl alloys using quantum mechanics/molecular mechanics simulations. We observe the magnetism-driven site preference of Fe and Co impurities at the dislocation core. When occupying the Ni sublattice, Fe and Co impurities are found to induce spontaneous dislocation cross slip. When occupying the Al sublattice, the impurities render the originally undissociated dislocation to split into two partials. Finally we observe the magnetism-driven dislocation mobility when Fe impurity occupies the Al sublattice, which has also been discovered experimentally. The magnetic interaction between the impurities and the host atoms is responsible for the significant changes in the dislocation core structure and mobility. DOI: 10.1103/PhysRevB.82.060404 PACS number͑s͒: 75.30.Hx, 61.72.Lk, 61.72.Nn, 71.20.Lp It has been shown experimentally that an applied magnetic field can change the plastic behavior of crystalline materials, a phenomenon known as magnetoplasticity.1,2 In a series of theoretical papers, Molotskii and Fleurov have explained the phenomenon by assuming that a dangling bond of a paramagnetic impurity forms a radical pair with a dangling bond of the dislocation core. They showed that the applied magnetic field could then induce transitions between different spin states of such pairs characterized by different binding energies, and thus facilitate dislocation depinning from the impurity and enhance the crystal plasticity.3 Despite its physical significance, the magnetoplasticity phenomenon becomes less relevant in most applications where materials deform in the absence of an applied magnetic field. However, a recent work combining theory and experiments 4,5 has shown that even in the absence of the magnetic field, magnetism plays an important role in the mechanical response of materials. In particular, it is discovered that 3d transitionmetal impurities ͑Fe, Co, Ni, Cr, etc.͒ could profoundly change the mechanical properties of B2-NiAl intermetallic alloys; the origin of the impurity-induced solid solution softening in these alloys is due to the magnetic interaction between the impurities and the host atoms. 6 The experimentally observed softening can only be reproduced by densityfunctional theory ͑DFT͒ calculations if the magnetic interaction ͑or spin polarization͒ is turned on. Similarly, the site preference and lattice spacing changes would switch sign if the spin polarization is turned off in the DFT calculations. These results along with the magnetoplasticity effect, highlight the important role that magnetism plays in the mechanical response of materials, illustrating the cross fertilization between two disciplines, magnetism and mechanical properties.B2 intermetallic NiAl alloys have attracted a lot of attention recently owing to their potential applications as hightemperature structural materials. One of the common practices to improve the mechanical properties of materials is alloying. For example, introducing substitutiona...