The development of stimuli-responsive chiral cholesteric liquid crystals (CLCs) materials holds significant potential for achieving three-dimensional (3D) anti-counterfeiting and multi-level information encryption. However, constructing phototunable CLCs systems with easy fabrication and fast response remains a great challenge. Herein, we exploit an excitation-dependent CLCs (ExD-CLCs) material by establishing dynamically photoresponsive dichroic competition between two achiral dyes: a negative dichroic dye (SP-COOH) and a positive dichroic dye (Nile Red, NR) within a CLCs medium. The ExD-CLCs exhibits a negative circularly polarized luminescence (CPL) signal (g