Atomistic modeling of materials failure is an introduction to molecular and atomistic modeling techniques applied to solid deformation and fracture. Focusing on a variety of brittle, ductile, and geometrically confined materials, this detailed overview includes computational methods at the atomic scale and describes how these techniques can be used to model the dynamics of cracks, dislocations, and other deformation mechanisms. A full description of molecular dynamics (MD) as a numerical modeling tool covers the use of classical interatomic potentials and the implementation of large-scale massively parallelized computing facilities, in addition to the general philosophies of model building, simulation, interpretation, and analysis of results. Readers will find an analytical discussion of the numerical techniques along with a review of required mathematical and physics fundamentals. Example applications are also included.