The thermosalient effect is a rarely observed, potentially very useful and at the present, unpredictable mechanical response during a phase transition that is thought to hold the potential for rapid and clean energy conversion devoid of gaseous products. Here, we report the serendipitous discovery of a rare instance of a thermosalient organic solid that exhibits the effect below room temperature. The crystals of this carbazole-based material are dynamic at both molecular and macroscopic scales. Using variable temperature synchrotron X-ray diffraction and variable-temperature solid-state nuclear magnetic resonance (ssNMR), we thoroughly examined the hysteretic structural transition in this material, emphasizing its macroscopic reconfigurability. We discovered unexpected large-amplitude molecular oscillations in the low-temperature phase, which challenge conventional assumptions about salient materials. Notably, we combined