Many order-disorder-type phase transitions in molecule-based ferroelectrics are related to changes of molecular dynamics. If the molecular motions do not involve reorientations of dipole moments, their ordering fails to contribute directly to spontaneous electric polarization. For understanding ferroelectric mechanisms in these systems, it is important to clarify how such molecular dynamics changes induce structurally symmetry-breaking phase transitions and thus the appearance of spontaneous electric polarization. Systematic characterization of an [18]crown-6 based host-guest inclusion compound, [(DIPA)([18]crown-6)]BF4 (DIPA = 2,6-diisopropylanilinium), shows it is an excellent ferroelectric with a large dielectric anomaly, significant pyroelectricity, and SHG response, and rectangular polarizaiton-electric field hysterisis loops. By the combination of variable-temperature single-crystal structural determination and solid-state NMR observation, it is found that the slowing down of the rotation of the [18]crown-6 molecule and the tumbling of the BF4 anion causes the symmetry breaking, while the spontaneous polarization is induced by the relative displacement between the cationic and anionic sublattices. This investigation will contribute to a deeper understanding of the structure-property relationship in the emerging molecular ferroelectrics.