The title compound, (Z)-4-(2-methoxybenzylidene)-1-methyl-2-phenyl-1H-imidazol-5(4H)-one (1), was synthesized and characterized. Compound 1 possesses two weak intramolecular C-H center dot center dot center dot O and C-H center dot center dot center dot N hydrogen bonds, which generate S(5) and S(6) rings, respectively. Intermolecular pi-pi stacking between the imidazolone ring and its adjacent one is observed in the crystal structure, which links a pair of molecules into a cyclic centrosymmetric dimer. Furthermore, two different C-H center dot center dot center dot pi interactions lead to the formation of columns along the [100] direction that are connected to one another via intermolecular C-H center dot center dot center dot O hydrogen bonds, so linking the molecules into a continuous three-dimensional framework. Its spectroscopic properties and complementary density functional theory calculations are also reported.