A novel ZnII complex bearing two monodentate (4-methoxyphenyl)[(1E, 2E)-3-phenylprop-2-en-1-ilidene] Schiff bases was synthesized and investigated both in the solid state by single-crystal X-ray diffraction, elemental analysis, and FTIR and in solution by 1H NMR spectroscopy. The complex crystallizes in the P21/c monoclinic space group. The asymmetric unit contains one ZnII ion coordinated to two Schiff base ligands and two chloride ions, in a distorted tetrahedral geometry. The title complex was also investigated by DFT, using the hybrid functional B3LYP with basis set 6-31G++, which reproduced the geometry and structural features of the complex in the crystal, and was used to assign the main bands in the FTIR spectrum. In solution, the complex maintains its integrity against decomposition to the parent reagents.