Growth of twin-free and high-quality 4-N,N-dimethylamino-4′-N′-methyl stilbazolium tosylate (DAST) crystals, with a surface roughness in the range of 1.7-3.8 nm (<4 nm) for as-grown crystals, has been achieved using solutions of lower supersaturation coupled with isothermal solvent evaporation. In addition, these efficient organic-ionic nonlinear optical (NLO) crystals possessed well-developed 001 and 001 h faces that facilitate direct utilization of these crystals for electrooptic (EO) and terahertz (THz) applications. Since this modified growth method necessitates a relatively lower amount (about 46%) of the expensive starting material as compared to that required for routine methods, it is also proven to be cost-effective.