This study investigated and evaluated a semi-active tuned mass damper which incorporated four multi-layered structures fabricated using magnetorheological elastomers. The four magnetorheological elastomer structures formed a square and provided the tuned mass damper variable stiffness used to track the excitation frequencies. This design not only increases the stability of the tuned mass damper but more importantly eliminates the magnetic circuit gap in a design which we used in the past because all four of the magnetic circuits used to control the magnetorheological elastomer isolators are closed circuits. In order to verify the capability of the magnetorheological elastomer-based tuned mass damper to protect a building from earthquake, extensive simulation and experimental testing were conducted. The swept sinusoidal signal and the scaled 1940 El Centro earthquake record were used to excite a scaled three-story building. Both simulation and experiment have verified that the magnetorheological elastomer-based tuned mass damper outperformed all other passive tuned mass dampers under either swept sinusoidal or seismic conditions.