A series of quinazolinone-based materials was synthesized and fully characterized. Firstly, the third-order nonlinear optical properties of the quinazolinone derivatives in CH2Cl2 were investigated by using Z-scan measurement. Secondly, the photophysical properties of the compounds were determined with aid of experimental and theoretical calculation methods. The results showed that the introduction of phenylacetylene groups on the planar structure of parent ring of 1a reduced the pi-pi intermolecular stacking of parent ring compound, and the formation of push-pull structure by connecting phenylacetylene groups to quinazolinone backbone decreased energy gap of entire molecule. A good NLO response was obtained, that the second-order NLO susceptibilities (gamma) of 2b were 6.225 x 10(-31) esu, which is more than 7 times higher than that of no-modified 1a. Our results indicate that the quinazolinone derivatives were promising candidate materials for future nonlinear optical applications.