The (E)-1-(4-methylbenzylidene)urea (EMBU) molecule have been synthesized and characterized by using FT-IR, FT-Raman and NMR spectral techniques. The quantum chemical calculations of EMBU have been done by using DFT/B3LYP/6- 31G(d,p) basis set. The bond parameters were calculated at same level of theory. The vibrational assignment of EMBU is assigned precisely with the help of potential energy distributions (PED). The hyperconjugative stabilizing interactions are studied by the natural bonding orbital (NBO) analysis. The NLO activity of EMBU is calculated and compared with the standard Urea molecule. The active sites were identified by the molecular electrostatic potential mapped surface. In addition, Mulliken atomic charges and thermodynamic properties were calculated and analyzed.