Novel organic nonlinear optical material pToluidinium malonate (PTM) was grown from aqueous solution by slow evaporation technique. The lattice parameters were evaluated from single crystal Xray diffraction analysis and found that crystal system belongs to monoclinic with centrosymmetric space group P2(1)c. The solid state parameters valence electrons, Plasma energy, Penn gap and Fermi energy were evaluated theoretically. These estimated values are used to calculate the electronic polarizability of PTM crystal. The functional groups exist in the compound were identified using FTIR and FTRAMAN spectroscopy. PTM crystal showed transmittance in the entire visible region with lower cut off wavelength of 311 nm and band gap energy of 3.8 eV. The photoluminescence spectrum was recorded to explore the emission and thermal behaviour of PTM crystal by employing TGDTA analysis. Dielectric measurement was carried out on the grown crystal at different temperatures to evaluate electrical properties. The thirdorder nonlinear optical parameters were estimated by Zscan technique using 532 nm diode pumped CW Nd:YAG Laser. (C) 2019 Elsevier B.V. All rights reserved.