Energy harvesting from vibrations is a popular research topic. However, it is difficult to change the values of its dynamic stiffness characteristics during the operation of device. This paper analyzes the nonlinear dynamical behavior and energy harvesting performance of an energy harvesting device with a gear unit and an inertial amplifier. The Melnikov method is used to discriminate the chaos behavior of the system and is illustrated by numerical simulations. Chaotic dynamics analysis provides a simplified analytical idea that offers more insight into the performance of this energy harvesting device. In addition, the basins of attraction of the coexistence solution of the system are plotted, and the trajectory and energy harvesting efficiency of the system are analyzed for changes in the initial value. The results show that the device has the convenience to change the form and efficiency of system energy harvesting. The theory of Melnikov functions recognizes the presence of chaos and can provide solutions for the parameterization of the system. The choice of initial value greatly affects the energy harvesting efficiency.