Relaxor ferroelectric Pb(Zn(1/3)Nb(2/3))O(3-x)PbTiO(3) (PZN-PT) and Pb(Mg(1/3)Nb(2/3))O(3)-PbTiO(3)(PMN-PT) single crystals are the potential candidates for future high-performance piezoelectric devices due to their exceptionally high dielectric and piezoelectric properties. Characterization on flux-grown PZN-PT single crystals of different orientations revealed that PZN-(6-7)%PT single crystals show good homogeneity in dielectric and electromechanical properties and composition. When poled in [001] direction, these crystals exhibit high longitudinal-mode properties with dielectric constant (K(T)) approximately equal to 7000, piezoelectric coefficients (d(33)) approximately equal to 2800 pC/N, and electromechanical coupling factors (k(33)) > or = 0.92. For [011]-cut crystals, optimally poled PZN-7%PT single crystal exhibits very high transverse-mode dielectric and piezoelectric properties with K(T) > or = 5000, d(32) approximately equal to -3800 pC/N and k(32) > or = 0.90. [011]- poled PZN 6%PT has d(32) approximately equal to -3000 pC/N and comparable k(32) and K(T) values. In comparison with melt-grown PMNPT single crystals, flux-grown PZN-PT single crystals show good compositional homogeneity, superior and consistent dielectric and electromechanical properties, and higher depolarization temperatures (TDP).