The dynamic control of circularly polarized luminescence (CPL) has far-reaching significance in optoelectronics, information storage, and data encryption. Herein, we reported the reversible inversion of CPL in a coassembly supramolecular system consisting of chiral molecules L4, which contain two positively charged viologen units, and achiral ionic surfactant sodium dodecyl sulfate (SDS) by introducing achiral sulforhodamine B (SRB) dye molecules. The chirality of CPL in the coassemblies can be efficiently regulated and inverted by simply adjusting the amount of SRB. A series of experimental characterization, including optical spectroscopy, electron microscope, 1 H NMR, and X-ray scattering measurements, suggested that SRB could coassemble with L4/SDS to establish a new stable L4/SDS/SRB supramolecular structure through electrostatic interactions. Moreover, the negative-sign CPL could revert to the positive-sign CPL if titanium dioxide (TiO 2 ) nanoparticles were used to decompose SRB molecules. The evolution of the CPL inversion process could be cycled at least 5 times without a significant decline in CPL signals when SRB was refueled to the system. Our results provide a facile approach to dynamically regulating the handedness of CPL in a multiple-component supramolecular system via achiral species.