A critical review of the physical and mechanical properties of NiAl is presented. The physical properties examined include electronic structure and bonding, crystal structure and phase stability, thermodynamic properties, elastic properties, and electrical, magnetic, and thermal properties. Discussion of crystal defects in NiAl include both constitutional and thermal point defects, the core structure and energy of line defects, and planar defects (shear faults, grain boundaries, and free surfaces). The mechanical properties, substructure, and mechanisms of ductility of NiAl single crystals and polycrystals are reviewed in detail, while alloying effects and the deformation of NiAl martensite are briefly described. The fracture toughness, modes of fracture, and cyclic properties reported in the literature are assessed. A critical analysis of diffusion data for NiAl is followed by a discussion of the activation energy and mechanisms of diffusion. This information is related to the creep properties of NiAl, and additional critical comments concerning the substructure and creep mechanisms of NiAl are provided. A review of the environmental resistance of NiAl is followed by a brief discussion of several current and potential applications of NiAl. Concluding remarks include suggestions for future research on NiAl.