Manganese (Mn)-copper (Cu)-based alloys have been found to havedamping capacity and can be used to reduce harmful vibrations and noise effectively. M2052 (Mn-20Cu-5Ni-2Fe, at%) is an important branch of Mn-Cu-based alloys, which possesses both excellent damping capacity and processability. In recent decades, lots of studies have been carried out on the performance optimization of M2052, improving the damping capacity, mechanical properties, corrosion resistance, and service temperature, etc. The major methods of performance optimization are alloying, heat treatment, pretreatment, and different ways of molding etc., among which alloying, as well as adopting a reasonable heat treatment, is the simplest and most effective method to obtain perfect and comprehensive performance. To obtain the M2052 alloy with excellent performance for casting molding, we propose to add Zn and Al to the MnCuNiFe alloy matrix and use a variety of heat treatment methods for a comparison in the microstructure, damping capacity, and service temperature. Thus, a new type of cast-aged Mn-22.68Cu-1.89Ni-1.99Fe-1.70Zn-6.16Al (at.%) alloy withsuperior damping capacity and high service temperature is obtained by an optimized heat treatment method. Compared with the forging technique, cast molding is simpler and more efficient, and the damping capacity of this as-cast alloy is excellent. Therefore, there is a suitable reason to think that it is a good choice for engineering applications.