With the rapid development of Internet of Things (IoT) and the popularity of wireless sensors, using internal permanent or rechargeable batteries as a power source will face a higher maintenance workload. Therefore, self-powered wireless sensors through environmental energy harvesting are becoming an important development trend. Among the many studies of energy harvesting, the research on rotational energy harvesting still has many shortcomings, such as rarely working effectively under low-frequency rotational motion or working in a narrow frequency band. In this article, a rotational magnetic couple piezoelectric energy harvester is proposed. Under the low-frequency excitation (<10 Hz) condition, the harvester can convert low-frequency rotational into high-frequency vibrational of the piezoelectric beam by frequency up-conversion, effectively increasing the working bandwidth (0.5–16 Hz) and improving the efficiency of low-speed rotational energy harvesting. In addition, when the excitation frequency is too high (>16 Hz), it can solve the condition that the piezoelectric beam cannot respond in time by frequency down-conversion. Therefore, the energy harvester still has a certain degree of energy harvesting ability (18–22 Hz and 29–31 Hz) under high-frequency conditions. Meanwhile, corresponding theoretical analyses and experimental verifications were carried out to investigate the dynamic characteristics of the harvester with different excitation and installation directions. The experimental results illustrate that the proposed energy harvester has a wider working bandwidth benefiting from the frequency up-conversion mechanism and frequency down-conversion mechanism. In addition, the forward beam will have a wider bandwidth than the inverse beam due to the softening effect. In addition, the maximum powers of the forward and inverse beams at 310 rpm (15.5 Hz) are 93.8 μW and 58.5 μW, respectively. The maximum powers of the two beams at 420 rpm (21 Hz) reached 177 μW and 85.2 μW, respectively. The self-powered requirement of micromechanical systems can be achieved. Furthermore, this study provides the theoretical and experimental basis for rotational energy harvesting.