Direct observations on nanopillars composed of molybdenum disulfide (MoS2) and chromium-doped MoS2 and their response to compressive stress have been made. Time-resolved transmission electron microscopy (TEM) during compression of the submicrometer diameter pillars of MoS2- and Cr-doped MoS2 (Cr: 0, 10, and 50 at %) allow the deformation process of the material to be observed and can be directly correlated with mechanical response to applied load. The addition of chromium to the MoS2 changed the failure mode from plastic deformation to catastrophic brittle fracture, an effect that was more pronounced as chromium content increased.