This paper investigated high-damping Cu-Al-Be-B cast alloys using metallographic analysis, X-ray diffraction (XRD) and electrical resistance measurements for transformation temperatures. The results showed that beryllium can stabilize β phase, resulting in a thermo-elastic martensite microstructure leading to high-damping capacity in cast Cu-Al-BeB alloys. Trace additions of boron to Cu-Al-Be alloys can significantly refine the grains, providing high strength and ductility to the alloys. A factorial design of experiment method was used to optimize the composition and properties of cast Cu-Al-BeB alloys. The optimal microstructure for thermo-elastic martensite can be obtained by adjusting the amounts of aluminum and beryllium to eutectoid or pseudo-eutectoid compositions. An optimized cast Cu-Al-Be-B alloy was developed to provide excellent mechanical properties, tensile strength σb = 767 MPa, elongation δ = 7.62 %, and damping capacity S. D.C =18.70%.