A novel technique of designing the interface layer in metal matrix composites of high damping capacity was developed via different CVD coatings on carbon fibers in Cf/Al composites. It was shown that the interface layer improved the tensile strength, elastic modulus and damping capacity of the Cf/Al composites. A carbon layer showed the highest improvement and a silicon layer the lowest, while a mixed carbon and silicon layer exhibited an intermediate effect. Moreover, the thickness of interface layer also influences the damping capacity. A thicker carbon layer produced a better damping capacity because the dependence of damping capacity on strain amplitude was increased. It is suggested that a micro-sliding action occurring in the interface layer is the main mechanism responsible for the high damping capacity of the composites.