Furthermore, we validate our findings by employing density functional theory(DFT) calculations to validate the ML-predicted refractive indices and hardness values. It is important to acknowledge a limitation of our approach, namely the inability to calculate SHG coefficients due to resource constraints directly. However, despite this limitation, several materials identified in our study have already been established as effective NLO substances in existing literature. We believe that the identified materials hold promise as potential NLO candidates.