A profound way to increase the output voltage (or power) of the piezoelectric nanogenerators is to utilize a material with higher piezoelectric constants. Here we report the synthesis of novel piezoelectric 0.72Pb(Mg(1/3)Nb(2/3))O(3)-0.28PbTiO(3) (PMN-PT) nanowires using a hydrothermal process. The unpoled single-crystal PMN-PT nanowires show a piezoelectric constant (d(33)) up to 381 pm/V, with an average value of 373 ± 5 pm/V. This is about 15 times higher than the maximum reported value of 1-D ZnO nanostructures and 3 times higher than the largest reported value of 1-D PZT nanostructures. These PMN-PT nanostructures are of good potential being used as the fundamental building block for higher power nanogenerators, high sensitivity nanosensors, and large strain nanoactuators.