In order to improve the vibration reduction performance of damping treatments, a new damping structure consisting of a uniform base layer and two periodically alternating free layers was examined in this study. Closed-form solutions for both the band structure and the forced response of the periodic bi-layer beam were theoretically derived and verified via numerical solutions using the finite-element method. The results showed that the structure with periodic free-layer damping (PFLD) treatment reduced broadband vibrations, and the levels of reduction were dominated by Bragg scattering in the band gaps and damping in the passbands. The vibration experiment verified the derived theory’s accuracy and showed that the PFLD treatment could increase vibration reduction levels in low-frequency band gaps compared with traditional free-layer damping treatments. The effects of the parameters—cell lengths, sub-cell-length ratios, and thickness ratios—were also discussed, providing further understanding of the vibration reduction performance of the bi-layer beam with the PFLD treatment, and this can be used to help designers optimize the periodic bi-layer beam to achieve better performance.