Optically good transparent quality of magnesium sulfate-doped adipic acid crystals was successfully grown by slow solvent evaporation route in methanol solvent at ambient temperature. The harvested crystal was crystallized in monoclinic crystal system with centrosymmetric space group P21/n. The measured size of the harvested crystal after a growth span of 14 days is 8 × 8 × 6 mm3. The determined second harmonic generation SHG efficiency of magnesium sulfate-doped adipic acid crystal is 2.63 times superior to that of pure adipic acid crystal. The high-resolution X-ray diffraction HRXRD experiment reveals that crystalline perfection of the grown crystal is optically good quality and consists of single diffraction peak. The obtained full width half maximum value (FWHM) of HRXRD diffraction curve is 40.07 arc second. The UV optical transmittance spectrum showed the band gap energy of 5.44 eV. FTIR and EDAX spectrum studies confirm the inclusion of dopant magnesium element into pure adipic acid host crystal matrix. The surface morphology of the grown crystal is platelet-like shape and confirms that the crystals have good crystalline nature. The grown crystal is thermally stable up to 107.3 °C. It is observed that magnesium sulfate-doped adipic acid crystal is softer than pure adipic acid sample.