Polymethyl methacrylate with Safranin O dye samples has been prepared using the severalweight percentage of the dye varying from 0.185 to 7.407 wt % of Safranin O. We have examined their structure, optical, dielectric and optical limiting properties. The preparation has been done utilizing a fast and simple method, casting technique, where both the polymer and the dye were solved in chloroform. The characterization of the structure has been achieved using XRD where the polymeric composites samples displayed a noncrystalline hump that supports the amorphous structure of the studied films. Spectroscopy measurements have been exhausted to approximate the spectral absorption estimations of the samples like absorbance, transmittance as well as the calculations of the index of absorption (k), and optical transition bandgap (Eg). The results indicate that the optical parameters alter by increasing the concentrations of the doping dye. From the obtained values of Eg, two optical transitions (direct and indirect) are possible for these composites. According to the applied models in the polymeric materials field, dielectric characterizations have been done and their parameters have been measured. We have studied the optical limiting characteristics of the samples with several concentrations of the dye using different laser sources of He–Ne working at 632.8 nm and 533 nm. The result showed an evident optical limiting impact on the films. Utilizing this optical limiting impact, the samples under consideration are appropriate to be applied in the applications of solar cell and CUT-OFF laser filters and laser power attenuation.