Thermosalient transitions are a subset of single-crystal-to-single-crystal (SCSC) transitions, in which the change of lattice parameters is highly anisotropic and very fast. As a result, crystals at the transition undergo macroscopic dynamical effects (hopping, jumping, and shattering). These transitions feature a conversion of heat to mechanical energy that can be exploited in the realization of advanced materials. Most thermosalient transitions are observed at temperatures higher than room temperature. Examples of low-temperature thermosalient transitions are rare. We describe a new example of a low-temperature thermosalient transition in a sexiphenyl compound. At about -40 °C, the parent single crystal (phase I) shatters into single crystal fragments of the new phase (phase II). The two phases have been studied by single-crystal X-ray analysis using a synchrotron source, variable-temperature Raman spectroscopy, and computational analysis of lattice normal vibration modes. A mechanism of the transition is proposed. We confirm colossal thermal expansion coefficients and supercells as reliable features of thermosalient transitions and add as a third feature a low-frequency principal optical vibration of the crystal lattice prompting the transition. Based on this, a roadmap for the automated prediction of thermosalient transitions in molecular crystals is also outlined.