PMMA is one of the most versatile polymeric materials for applications in various technological areas including optics and electro-optics. While the current applications of PMMA in optics and electro-optics are limited by their linear optical behavior, we report here in this paper the unique nonlinear optical behavior of nanohybrids consisting of nanocrystalline TiO2 in PMMA. Transparent thin films of TiO2-PMMA nanohybrid on substrates were synthesized by in-situ sol-gel and polymerisation, assisted by spin coating. Using titanium isoproproxide (Ti-iP) as the starting material for nanocrystalline titania, together with methyl methacrylate and 3-(trimethoxysilyl)propyl methacrylate, nanohybrids containing up to 80% Ti-iP in PMMA were successfully realized. The resulting nanohybrid thin films coated on quartz substrates are optically transparent and demonstrate large nonlinear optical behavior, with an ultrafast response of <1.5 ps. The highest two-photon absorption coefficient (β) and nonlinear refractive index (n2) are observed with the nanohybrid thin film of 60 wt% Ti-iP in PMMA, as confirmed by the Z-scan technique.