The 2‐methyl‐4‐nitroaniline (NA) was converted into the raw material N‐benzyl‐2‐methyl‐4‐nitroaniline (BNA), and the solubility of BNA in various organic solvents was calculated gravimetrically. BNA's solubility and crystal structure make it an excellent solvent for the low‐temperature solution growth method used to create single crystals of BNA with orthorhombic structure studied through single crystal analysis. Methanol was used to harvest the 3×10 mm3 BNA single crystals, which are big, translucent yellow crystals. BNA, the subject compound, the exothermic and endothermic nature was characterised by TG analyses, differential scanning calorimeter (DSC), functional studies by infrared (IR) spectra, NMR spectral and optical transmission studies. An Nd:YAG laser (1064 nm) was used to observe the second harmonic generation (SHG) of grown crystal leads about 3 times more than KDP crystal. Possible polarization for various temperatures, the crystal's dielectric properties was measured as a function of frequency. Larger surface morphology with high optical to wave conversion efficiency and the results were reviewed. Responding to electric field to leads to liquid crystal display and THz purposes.