We perform atomistic simulations of nanoindentation on Lennard–Jones 2D hexagonal crystals. In this work, we find a new spatially extended buckling-like mode of instability, which competes with the previously known instability governed by dislocation-dipole nucleation. The geometrical parameters governing these instabilities are the lattice constant, a, the radius of curvature of the indenter, R, and the thickness of the indenter layer, Ly. Whereas dislocation nucleation is a saddle-node bifurcation governed by R/a, the buckling-like instability is a pitchfork bifurcation (like classical Euler buckling) governed by . The two modes of instability exhibit strikingly different behaviors after the onset of instability. The dislocation nucleation mode results in a stable final configuration containing a surface step and a stable dislocation at some depth beneath the surface, while the buckling modes are always followed immediately by subsequent nucleation of many dislocation dipoles. We show that this subsequent dislocation nucleation is also observed immediately after buckling in free standing rods, but only for rods which are of sufficiently wide aspect ratio, while thinner rods exhibit stable buckling followed only later by dislocation nucleation in the buckled state. Finally, we study the utility of several recently proposed local and quasi-local stability criteria in detecting the buckling mode. We find that the so-called Λ criterion, based on the stability of a representative homogeneously deformed lattice, is surprisingly useful in detecting the transition from dislocation-type instability to buckling-type instability.