In this paper, we present a novel vibration-based piezoelectric energy harvester, capable of collecting power at multiple operating frequencies and autonomously adapting itself to the dominant ambient frequencies. It consists of a compact dual-frequency resonator designed such that the first two fundamental natural frequencies are in the range of [50, 100] Hz, which is a typical frequency range for ambient vibrations in industrial environments. A magnetic frequency-tuning scheme is incorporated into the structure, which enables the frequency agility of the system. In contrast to single frequency harvesters, the presented approach combines multi-resonance and frequency tunability of both modes enabling a larger operative bandwidth. We experimentally demonstrate independent bi-directional tunability of our dual-frequency design. Furthermore, a control algorithm based on maximum amplitude tracking has been implemented for self-adaption of the system. The latter has been demonstrated in a system-level simulation model, which integrates the dual-frequency resonator, the magnetic tuning, and the control algorithm.