A new class of vibration energy harvester based on magnetostrictive material (MsM), Metglas 2605SC, is designed, developed and tested. It contains two submodules: an MsM harvesting device and an energy harvesting circuit. Compared to piezoelectric materials, the Metglas 2605SC offers advantages including higher energy conversion efficiency, longer life cycles, lack of depolarization and higher flexibility to survive in strong ambient vibrations. To enhance the energy conversion efficiency and alleviate the need of a bias magnetic field, Metglas ribbons are transversely annealed by a strong magnetic field along their width direction. To analyze the MsM harvesting device a generalized electromechanical circuit model is derived from Hamilton's principle in conjunction with the normal mode superposition method based on Euler–Bernoulli beam theory. The MsM harvesting device is equivalent to an electromechanical gyrator in series with an inductor. In addition, the proposed model can be readily extended to a more practical case of a cantilever beam element with a tip mass. The energy harvesting circuit, which interfaces with a wireless sensor and accumulates the harvested energy into an ultracapacitor, is designed on a printed circuit board (PCB) with plane dimension 25 mm × 35 mm. It mainly consists of a voltage quadrupler, a 3 F ultracapacitor and a smart regulator. The output DC voltage from the PCB can be adjusted within 2.0–5.5 V. In experiments, the maximum output power and power density on the resistor can reach 200 µW and 900 µW cm⁻³, respectively, at a low frequency of 58 Hz. For a working prototype under a vibration with resonance frequency of 1.1 kHz and peak acceleration of 8.06 m s⁻² (0.82 g), the average power and power density during charging the ultracapacitor can achieve 576 µW and 606 µW cm⁻³, respectively, which compete favorably with piezoelectric vibration energy harvesters.