The colloidal silica was modified with 3-aminopropyltrimethoxysilane (APTES), and then further treated with photosensitive polyurethane based NCO-terminated oligomers to yield photosensitive polyurethane modified silica. Polyurethane acrylate (PUA) nanocomposite films were prepared with incorporation of the surface treated silica. IR and TGA results confirm the existence of PU oligomer at the surface of silica. TEM and SEM analysis shows that the PU-silica uniformly disperses in toluene and polyurethane matrix. Rheology, DMA and stress-strain analysis demonstrate that the evidence of the stronger interfacial interactions between the oligomer molecules at the surface of silica and polyurethane matrix. The PU-silica functionalized nanocomposite films display enhanced elastic modulus, storage modulus and tensile strength.