A novel organic nonlinear optical (NLO) compound (2E)-3-(2-methylphenyl)-1-(4-nitrophenyl) prop-2-en-1-one (2MPNP) has been synthesized and grown as a high-quality single crystal by the slow evaporation technique. 2MPNP crystals were characterized by FT-IR, UV-Vis-NIR, NMR, DSC, and Single Crystal XRD techniques. 2MPNP crystallizes in the orthorhombic crystal class in the noncentrosymmetric space group Pca2(1) with cell parameters a = 29.905(4) angstrom, b = 4.8241(5) angstrom, c = 9.0984(10) angstrom, alpha = beta = gamma = 90.00 degrees, and V = 1312.58 angstrom(3) and Z = 4. Second harmonic generation (SHG) efficiency of the grown crystal was found to be 1.17times that of urea. Thermal analysis reveals that the crystal has better thermal stability.