This paper reports the high-temperature top-seeded solution growth (TSSG) of large single crystal of Nd3+-doped GdAl3(BO3)(4) from a K2Mo3O10-LiF flux cooled at a rate of 2 K/day and using a crystal rotation rate of 4.5 rpm. The polarized optical absorption and fluorescence spectra of Nd3+ : GdAl3(BO3)(4) crystal have been investigated. Polarized absorption cross sections are 4.3 x 10(20) and 2.6 x 10(20) cm(2) with band widths of 8.7 and 6.1 nm for sigma- and pi -polarization, respectively. The emission cross sections are 6.3 x 10(-19) and 6.0 x 10(-19) cm(2) for sigma- and pi -polarization, respectively, at 1062 nm corresponding to the F-4(3.2)--> I-4(112) transition. The fluorescence lifetime is 54.3 and 57 mus at 300 and 20 K, respectively.