Two ferroelectric single crystals Pb0.37Ba0.63 Nb2O6 and Pb0.30Ba0.533Na0.306Li0.028 Nb2O6,pulled from melt by Czochralski technique, have been studied. By X-ray diffraction, it has been determined that both of two crystals belong to the tetragonal system with lattice parameters a = 12.493 ?, c = 3.984 ? for PBN, and a = 12.493 ?, c=3.970 ? for Li, Na-doped PBN. All of the dielectric, elastic, and piezoelectric coefficients of the two crystals have been measured. The results show that PBN crystal possesses good piezoelectric character with d15≈108×10-12C/N. This crystal could be a promising material for piezoelectric transducers operating in the shear mode. The dielectric constants are reduced, while the Tc is enhanced obviously in PBN doped by Li and Na Ions.