The effect of shear strain on the high‐pressure behavior of nitromethane has been studied by Raman spectroscopy in a shear diamond anvil cell (SDAC). Two major effects of shear strain have been observed. The first one is a lowering of the pressures at which the different spectral transformations occur. The second effect is observed at 28 GPa. At this pressure, a sudden decomposition of the sample occurs due to the shear deformation. Observation of the sample after decomposition shows the presence of a black residue, which is mainly composed of carbon soot.