Based on the anionic group theory [1-2], a computer-assisted material design system (CAMDS) has been develop and show to be a highly efficient means for discovering nonlinear optical crystals. In this method, important optical properties of the target compounds (borates, for example), such as the d(ij) coefficients, refractive indices and energy bandgap, are calculated so that a prior evaluation can be made before experiments. The results have given a meaningful guide to ensuring experiments, which have led to our discoveries of KBBF (KBe2BO3F2) and SBBO (Sr2Be2B2O7) in previous years followed by other members of the SBBO family in recent years. On the other hand, the system can also be used to evaluate the d(ij) coefficients of the berate NLO crystals discovered recently whose d(ij) coefficients have not been determined from experiment.