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A new chiral bromobinaphthol-pyrene compound was developed to achieve a green circularly polarized luminescence (CPL) from its excimer with a dissymmetry factor (|glum|) value of 4.3×10×3 and a high quantumyieldΦ F, solid up to 55.9％, while no CPL signals could be observed for the blue luminescence from unimolecule. Meanwhile, reversal CPL signals can be observed from both concentrated solution and solid.