  We report a systematic investigation on the magnetization relaxation
properties of iron-based half-metallic Heusler alloy
Fe$_{2}$Cr$_{1-x}$Co_${x}$Si (FCCS) thin films using broadband angular-resolved
ferromagnetic resonance. Band structure engineering through Co doping (x)
demonstrated by first-principles calculations is shown to tune the intrinsic
magnetic damping over an order of magnitude, namely 0.01-0.0008. Notably, the
intrinsic damping constants for samples with high Co concentration are among
the lowest reported for Heusler alloys and even comparable to magnetic
insulator yttrium iron garnet. Furthermore, a significant reduction of both
isotropic and anisotropic contributions of extrinsic damping of the FCCS alloys
was found in the FCCS films with x=0.5-0.75, which is of particular importance
for applications. These results demonstrate a practical recipe to tailor
functional magnetization for Heusler alloy-based spintronics at room
temperature
