More effective organic charge transfer nonlinear optical material of 2-(4-methlybenzylidene) malononitrile (MBM) has been synthesized via knoevenagel condensation reaction method and single crystals of unprecedented MBM were successfully cultivated in the presence of ethanol solution by the adaption of slow evaporation solution growth method. Cell parameters and phase purity of the obtained MBM crystals were investigated with the help of Single crystal and powder X-ray diffraction analysis. The morphology of the grown crystal was generated using WinXMorph software. Linear optical characterization was carried out in order to figure out its transmittance efficiency (82%), cut-off wavelength (λ = 458 nm) and energy band gap (Eg = 3.05eV) of the title material. Electrical behavior of the MBM crystal was examined on the basis of dielectric properties. Title crystals thermal tolerance and melting point was examined through TG-DSC analysis. The grown MBM crystal was subjected to Single beam Z-scan technique in order to figure out its third order nonlinear optical nature and its susceptibility is compared with other reported centrosymmetric crystals. Considering its large transmittance range, thermal stability and effective NLO performance, MBM is a potential candidate for NLO applications. © 2020 Elsevier B.V.