The high quality crystals of GdAl_3(BO_3)_4:Nd3+ with the sizes of 35mm have been grown from K2Mo3O10-B2O3 solvent system.The a and π polarization absorption and edrission spectra of GdAl3(BO3)4:Nd3+ have been measured. A laser output of 119.5μＪ at 0.532 μm with an optical to optical efficiency of 4.3% was obtained by using self-frequency doubling technology when this crystal was pumped by dye laser. Also, a laser output of 445μJ at 436－443 nm range with an optical to optical efficiency of 7.3% was obtained by using self sum frequency method when this crystal was pumped by dye laser.