The existence of a correlation between spin crossover and dielectric properties is a hot topic in the field of multiresponse materials, which has potential applications in the memory devices, switches, and sensors. One formidable challenge is the simultaneous and rapid on/off switching of spin states of the spin carriers and magnetic coupling between them, which is crucial for both reversible photo magnetic behavior and variations in dielectric properties. Here, we report a dinuclear Fe(II) spin crossover complex, wherein each Fe(II) center exhibits an interconversion between Fe-HS(II) (HS = high-spin) and Fe-LS(II) (LS = low-spin) achieved upon heating and cooling. Moreover, the spin state of respective Fe(II) ions and the antiferromagnetic interaction between them can be switched bidirectionally under alternating irradiation with 532 and 808 nm light, resulting in interconversion between paramagnetic and diamagnetic properties. Interestingly, the spin crossover can also induce variations in dielectric tensors. This result provides a strategy to simultaneously and bidirectionally switch spin state, magnetic coupling, and dielectric properties using external stimuli.