This work investigated the electromechanical performance of a cantilevered vibration energy harvester incorporating the single crystal PMN-PZT, manufactured with the most recent technology of solid-state single crystal growth. The performances of single crystal PMN-PZTs with two different crystallographic axes such as [011] and [001] are compared with those of PZT ceramics. From the investigations, it is shown that the [001]-poled PMN-PZT is advantageous for the excitations containing single dominant frequency component, while the single crystal [011]-$d_{32}$ is superior in terms of the energy storage density and energy conversion efficiency.