The title compound, 5-ethoxycarbonyl-4-[(4-methoxycarbonyl)phenyl]-6-methyl-3,4-dihydropyrimidin-2(1H)-ones (1), was synthesized from the one-pot, three-component condensation reactions and characterized by FTIR, H-1 NMR, HRMS, and single crystal X-ray diffraction. The compound (1) crystallizes in a triclinic system, space group P-1 with a = 6.1874(12), b = 7.5715(15), c = 17.369(4)angstrom, alpha = 80.24(3), beta = 81.15(3), gamma = 76.93(3)degrees, and Z = 2. The molecules are linked by hydrogen bonds N-H center dot center dot center dot O and C-H center dot center dot center dot O to generate a 2D network. In addition, UV-visible and fluorescence spectral measurements prove that it shows positive solvatochromic effect as the solvent polarity was increased.