With the rapid advance of laser technology in the photonicera, damage to precision optical instruments caused by exposure to sudden intense laser pulses has stimulated the search for effective optical power limiting materials exhibiting good dispersion, fast response speed, and good visible light transparency. In this study, novel binary Ni-based mixed MOF NSs (M = Mn, Zn, Co, Cd, Fe) were obtained, making the electronic transition more selective and changing the band gap to obtain an excellent reverse saturation absorption signal. The theoretical calculation results show that with the doping of the Fe element, the band gap of Ni-MOF NSs decreases from 3.12 to 0.66 eV of Ni-Fe-MOF NSs, indicating that the doping of the Fe element has a positive effect on the reverse saturated absorption. The experimental results prove that the optical limiting threshold of Ni-Fe-MOF NSs is better than the GNSs, indicating that the Ni–Fe-MOF NSs have a broad application prospect in the field of nonlinear optics and photonics.