Single crystals of Gd1-xRxCa4O(BO3)(3) (R3+ = Sc3+ or Lu3+) with large size and good quality have been grown by Czochralski method. The chemical compositions of the grown crystals were determined and X-ray diffraction measurements have been carried out to characterize the structural changes with compositional parameter x. The solubility limits of R3+ ions in the Gd4Ca4O(BO3)(3) crystals were also determined. Type-I noncritical phase-matching wavelengths for second-harmonic generation in Gd1-xRxCa4O(BO3)(3)-grown crystals were measured and compared with theoretical predictions. (c) 2006 Elsevier B.V. All rights reserved.