The proposed novel optical system of composites of polymethyl methacrylate (PMMA)/titanium oxide (TiO2) nanoparticles were planned to be used as polymeric materials according to their standing full applied optical applications. The spin coating method, an easy and cost-effective technique, was utilized to uniformly deposit and prepare these TiO2/PMMA thin films on glass substrates, wherein nature, the films’ uniformity, and structures’ crystallinity. The interactions between the TiO2 nanoparticle and PMMA as a matrix were confirmed through atomic force microscopy (AFM) and x-ray diffraction (XRD). The linear optical characterization of the obtained thin films was characterized using a spectrophotometer at a wavelength ranging from 200 nm to 1000 nm. Linear refractive index and absorption coefficient, direct and indirect optical bandgaps, and nonlinear optical parameters for the as-prepared samples were calculated using Kramers-Kroning analysis. Moreover, the optical limiting was studied using He-Ne laser 632.8 nm and green diode laser with 532 nm wavelength. This TiO2/PMMA, as a novel optical system, is a good optical system to be used for capable various future technical applications, such as optical filter, solar cells, electronic apparatus, and optoelectronics devices.