Molecular motions are essential natures of matters, and play important roles in their structures and properties. However, owing to the diversity and complexity of structures and behaviors, the study of motion-structure-property relationship remains a challenge, especially at all levels of structural hierarchy from molecule to macro-object. Herein, luminogens showing aggregation-induced emission (AIE), namely 9-(pyrimidin-2-yl)-carbazole (PyCz) and 9-(5-R-pyrimidin-2-yl)-carbazole; R = Cl (ClPyCz), Br (BrPyCz) and CN (CyPyCz) were designed and synthesized, to decipher the dependence of materials' structures and properties on molecular motions at molecule and aggregate levels. Experimental and theoretical analysis demonstrated that the active intramolecular motions in the excited state of all molecules at single molecule level imparted them with more twisted structural conformations and weak emission. However, owing to the restriction of intramolecular motions in the nano/macro aggregate state, all the molecules assumed less twisted conformations with bright emission. Unexpectedly, intermolecular motions could be activated in the macro crystals of ClPyCz, BrPyCz and CyPyCz through the introduction of external perturbations, and synergic strong and weak intermolecular interactions allowed their crystals to undergo reversible deformation, which effectively solved the problem of the brittles of organic crystals, meanwhile imparted them with excellent elastic performance. Thus, the present study provided insights on the motionstructure-property relationship at each level of structural hierarchy, and offered a paradigm to rationally design multifunctional AIE-based materials.