Impact toughness is essential for evaluating the mechanical properties of ship hull steels. This study focused on understanding the embrittlement mechanism of NiAl precipitation-strengthened HSLA steels by integrating advanced characterization and atomic-scale calculations. The factors causing the deterioration of the impact toughness of NiAl precipitation-strengthened steels, which have been contentious, were identified. The embrittlement mechanism and crack propagation mode were revealed using first-principles calculations and 3D impact fracture morphology, respectively. The results suggested that the numerous homogeneous NiAl nanoparticles within the bcc-Fe matrix reduced the impact toughness of the HSLA steels. As the precipitate interparticle spacing (L) decreased, the impact toughness decreased until it attained a critical value (similar to 27 nm). This is interpreted effectively by the calculations indicating that the shear modulus (75 GPa) and fracture energy (4.5 J/m(2)) of the NiAl phase, particularly the NiAlMn phase (46 GPa, 4 J/m(2)), are significantly lower than those of bccFe (83 GPa, 5 J/m(2)). This induces the fracture of nanoparticles under rapid impact loading, which functions as numerous crack initiations before plastic deformation of the matrix. The small L achieved after peak-hardening aging can result in the interconnection of these crack sources and cause instantaneous cleavage fractures, similar to brittle materials.