The investigation of nonlinear optical (NLO) properties is crucial for the effective application of CsPbI 3 /TiO 2 nanocomposites in NLO devices. The CsPbI 3 /TiO 2 nanocomposites were synthesized by a hot injection method. Then, the CsPbI 3 /TiO 2 nanocomposites were poured into methyl methacrylate via polymerization to fabricate CsPbI 3 /TiO 2 /PMMA organic glasses (OGs). The crystal structure and size morphology of the CsPbI 3 /TiO 2 nanocomposites were examined using X-ray diffraction (XRD) and transmission electron microscopy (TEM), respectively. The nonlinear absorption (NLA), nonlinear refraction (NLR), and optical limiting (OL) properties of the CsPbI 3 /TiO 2 /PMMA OGs were investigated by using the Z-scan technique, employing a nanosecond pulse laser operating at a wavelength of 532 nm. The CsPbI 3 /PMMA and CsPbI 3 / TiO 2 /PMMA OGs can be transferred from saturable absorption (SA) to reverse saturable absorption (RSA) by varying the incident energy. In addition, the CsPbI 3 /TiO 2 /PMMA OGs exhibit superior NLA, NLR, and OL performances compared to the CsPbI 3 /PMMA OG and other halide-based perovskites. The enhanced nonlinear optical (NLO) properties of CsPbI 3 /TiO 2 /PMMA OGs can be ascribed to the cooperative interaction between CsPbI 3 and TiO 2 . In summary, the results indicate that CsPbI 3 /TiO 2 nanocomposites possess substantial potential for applications in NLO devices such as optical limiters, optical switches, and optical modulators.