The low-temperature phase, trigonal phase, of space group R32 was discovered in the compound LaSc3(BO3)4 (LSB) doped with arbitrary concentration of Nd3+ ions (NLSB). For LSB, the lattice constants are a = 9.820 ± 0.003 Å, c = 7.975 ± 0.003 Å. The decomposition of NLSB phase was observed in two regions of temperature below and above the congruent melting point by differential thermal analysis and x-ray powder diffraction methods. The single crystals of 2 × 2 × 3mm3 of dominant trigonal phase for x = 0.5 were grown by the flux method (LiBO2). Second harmonic generation effect was observed in NLSB for x = 0 to 1. The concentration dependence of fluorescence lifetime was measured and derived from Dexter's theory of resonant energy transfer.