Vibrational energy harvesting has attracted considerable research attention for electrical power collection from ambient vibrations. Thereby, this study first developed an electromagnetic energy harvester of large-scale bistable motion by application of stochastic resonance, to enhance energy harvesting efficiency at a broadly low frequency. The electromagnetic energy harvester is fabricated by a magnet-coil generator and an oblique-supported spring-mass system. In the beginning, a weighting function is originally proposed considering mutual position relationship of the magnet and coil, and a motion equation and an electromagnetic induction equation are simultaneously established considering both elastic spring recovery force and electromagnetic induction Lorentz force. Subsequently, numerical analysis is processed to resolve the simultaneous equations to obtain systematic response displacement and the induced voltage, and the numerical solutions are accurately consistent with the measuring results in validation experiments. Furthermore, a damping coefficient is identified considering the mutual effectiveness of the damping forces from the normal friction and electromagnetic induction, and the influence of electromagnetic induction damping on systematic response displacement is carefully discussed. Eventually, experimental results clarified that the stochastic resonance phenomenon actually occurred as a large-scale bistable motion, and it is further validated that power generation efficiency can be noticeably enhanced following amplitude amplifications of systematic response displacement.