The poling responses of [011]-poled Pb(Zn 1=3 Nb 2=3 )O 3 -PbTiO 3 [PZN-PT] single crystals of a range of compositions and two length orientations have been investigated. The results show that [011]-poled PZN-PT single crystals of [100]-length-cut exhibit much superior transverse properties than [01 1 1]-length-cut crystals. Extremely high d 31 values of Àð3000 { 4000Þ pC/N and k 31 $ 0:90 { 0:96 were obtained for PZN-7%PT optimally [011]-poled crystals. This composition, however, shows degraded dielectric and piezoelectric properties when poled at !0:6 kV/mm. In contrast, PZN-4.5%PT and PZN-6%PT single crystals show no signs of overpoling even when poled up to 2.0 kV/mm, exhibiting d 31 % Àð2700 { 3200Þ pC/N and k 31 $ 0:90 { 0:92 (for PZN-6%PT) and d 31 % À1500 pC/N and k 31 $ 0:86 { 0:90 (for PZN-4.5%PT), respectively. The presence of certain amounts (i.e., 10 -15%) of orthorhombic phase in a rhombohedral matrix has been found to be responsible for the superior transverse piezoelectric properties of optimally [011]-poled PZN-(6 -7)%PT.