Large crystals of Nd3+ : GdAl3(BO3)(4) with size up to 35 mm have been grown from a K2Mo3O10-B2O3 solvent. The liquid temperature curve for this growth system was determined by repeated seeding. From the grown crystal boule, a high-quality laser bulk crystal with dimensions of 4 mm x 5 mm x 6 mm was cut out, the absorption spectrum and the refractive indices of NGAB crystal as well as its temperature coefficients were measured. The phase-matching angles have been calculated. A laser output of 5 mW at 0.532 mu m with an optical to optical efficiency higher than 0.5% has been realized when this crystal was pumped by a GaAlAs laser diode.