Herein, a chiral charge transfer crystal that exhibits reversible phase transition between chiral space groups has been fabricated. When the phase switches from left-handed to right-handed chiral space group, more pronounced orbital angular momentum will be generated, where magneto-responsive optics are opposite for chiral enantiomers. Moreover, circularly polarized light could enhance the chiral orbit of the crystal with the same spiral orientation to let spin have a better ability to resist external magnetic field. Thus, magnetic field dependence of transmission and photoluminescence of chiral crystals are strongly dependent on the polarized state of incident light. Furthermore, through studying the coupling among spin, orbit, and circular photon, we obtained that the chiral orbit plays a key role for the coupling between the spin and circular photon. It is expected that this work could promote further exploration of organic chiral magneto-optical crystals in potential applications of sensing.