4-Methyl anilinium phenolsulfonate single crystal has been synthesized and grown by the slow evaporation solution technique at room temperature using methanol as a solvent. The crystal structure of the grown crystal was determined by the single crystal X-ray diffraction method. The various functional groups present in the crystal, and the different types of protons and carbons have been identified by the FT-IR and NMR spectral analyses respectively. Optical properties were determined by UV-vis-NIR spectroscopic and photoluminescence studies. The thermal and mechanical stabilities of 4-methyl anilinium phenolsulfonate single crystal have been investigated by TGA/DTA and Vickers microhardness measurements respectively. (C) 2013 Elsevier B.V. All rights reserved