Power source is critical to achieve independent and autonomous operations of electronic mobile devices. The vibration-based energy harvesting is extensively studied recently, and recognized as a promising technology to realize inexhaustible power supply for small-scale electronics. Among various approaches, the piezoelectric energy harvesting has gained the most attention due to its high conversion efficiency and simple configurations. However, most of piezoelectric energy harvesters (PEHs) to date are based on bending-beam structures and can only generate limited power with a narrow working bandwidth. The insufficient electric output has greatly impeded their practical applications. In this paper, we present an innovative lead zirconate titanate (PZT) energy harvester, named high-efficiency compressive-mode piezoelectric energy harvester (HC-PEH), to enhance the performance of energy harvesters. A theoretical model was developed analytically, and solved numerically to study the nonlinear characteristics of the HC-PEH. The results estimated by the developed model agree well with the experimental data from the fabricated prototype. The HC-PEH shows strong nonlinear responses, favorable working bandwidth and superior power output. Under a weak excitation of 0.3 g (g = 9.8 m/s2), a maximum power output 30 mW is generated at 22 Hz, which is about ten times better than current energy harvesters. The HC-PEH demonstrates the capability of generating enough power for most of wireless sensors.