Piezoelectric nanocomposites represent a unique class of materials that synergize the advantageous features of polymers and piezoelectric nanostructures and have attracted extensive attention for the applications of energy harvesting and self-powered sensing recently. Currently, most of the piezoelectric nanocomposites were synthesized using piezoelectric nanostructures with relatively low piezoelectric constants, resulting in lower output currents and lower output voltages. Here, we report a synthesis of piezoelectric (1 - x)Pb(Mg1/3Nb2/3)O3-xPbTiO3 (PMN-PT) nanowire-based nanocomposite with significantly improved performances for energy harvesting and self-powered sensing. With the high piezoelectric constant (d33) and the unique hierarchical structure of the PMN-PT nanowires, the PMN-PT nanowire-based nanocomposite demonstrated an output voltage up to 7.8 V and an output current up to 2.29 μA (current density of 4.58 μA/cm(2)); this output voltage is more than double that of other reported piezoelectric nanocomposites, and the output current is at least 6 times greater. The PMN-PT nanowire-based nanocomposite also showed a linear relationship of output voltage versus strain with a high sensitivity. The enhanced performance and the flexibility of the PMN-PT nanowire-based nanocomposite make it a promising building block for energy harvesting and self-powered sensing applications.