In this work, we designed a new kind of chiral organogold(I) luminophore species featuring moieties capable of rotational motion, with the aim of achieving thermo-responsive CPL properties that can be modulated by molecular rotation within the crystal (Figure ). To this end, binuclear Au(I) complexes, 1-R and 1-S, with chiral N-heterocyclic carbene (NHC) ligands featuring phenyl rotator moieties at the chiral centers, were synthesized and studied. In the crystalline state, these complexes exhibit a distinct chiral conformation with C2 symmetry, derived from non-equivalent orientations of phenyl moieties at the chiral centers of NHC ligands. In addition, according to the results of the variable-temperature solid-state 2 H NMR study, these nonequivalent phenyl moieties undergo rotational motion above 273 K. In line with our expectations, the presence of inherent chirality, luminescence, and thermally activated rotational motion in the crystalline state of the studied complexes resulted in the emergence of thermo-responsive CPL properties, with CPL intensity (ΔICPL) and luminescence dissymmetry factors (glum) showing a noticeable increase upon cooling from 333K to 213K (|ΔICPL|: + ~300%; |glum|: + ~50%). This behavior is attributed not only to rotation-induced luminescence quenching but also to the rotation effect on the symmetry of the complexes, thereby affecting the glum values.