The optical birefringence of Gd1-xRxCa4O(BO3)(3) (R = Lu or Sc) crystals can be controlled by changing the compositional parameter x. Two nonlinear crystals of Gd0.884Lu0.116Ca4O(BO3)(3) and Gd0.952Sc0.048Ca4O(BO3)(3) with large size and good quality have been grown by Czochralski method. According to our assumptions, the obtained results demonstrate that both crystals convert the near-infrared radiation of 800nm into blue-violet light (400nm) by type-I noncritical phase-matching (NCPM) second-harmonic generation (SHG) processes along Y axis.