Self-powered nanodevices scavenging mechanical energy require piezoelectric nanostructures with high piezoelectric coefficients. Here we report the fabrication of a single-crystal (1 - x)Pb(Mg1/3Nb2/3)O3 - xPbTiO3 (PMN-PT) nanobelt with a superior piezoelectric constant (d33 = ~550 pm/V), which is approximately ~150%, 430%, and 2100% of the largest reported values for previous PMN-PT, PZT and ZnO nanostructures, respectively. The high d33 of the single-crystalline PMN-PT nanobelt results from the precise orientation control during its fabrication. As a demonstration of its application in energy scavenging, a piezoelectric nanogenerator (PNG) is built on the single PMN-PT nanobelt, generating a maximum output voltage of ~1.2 V. This value is ~4 times higher than that of a single-CdTe PNG, ~13 times higher than that of a single-ZnSnO3 PNG, and ~26 times higher than that of a single-ZnO PNG. The profoundly increased output voltage of a lateral PNG built on a single PMN-PT nanobelt demonstrates the potential application of PMN-PT nanostructures in energy harvesting, thus enriching the material choices for PNGs.