To respond to the gradually increasing demand for thermal stability of sintered NdFeB magnets and grasp the evolution rules of their phase structure, research on sintered Nd-Dy-Fe-Co-B magnets was conducted. The magnets used in this study were prepared by the powder metallurgy method (Strip Casting + Hydrogen Decrepitation + Jet Milling). The room temperature magnetic properties of the magnet sample were Br = 11.45 kGs and Hcj = 22.42 kOe, with a low-temperature coefficient of Br (αBr(20 °C∼100 °C) = −0.059 %/°C) and a high Curie temperature (Tc = 460 °C). Based on the microstructure observation, there were planar anisotropic soft magnetic phase Nd2Co17 within grain boundaries and the "Cu-Co Opposite Distribution". Low-melting-point binary alloy Pr80Cu20 was introduced into the magnet by grain boundary addition to eliminate Nd2Co17 phases and improve the coercivity. After the grain boundary addition, the "Cu-Co Opposite Distribution" was used to eliminate the Nd2Co17 phase, the grain boundary structure was optimized, and the coercivity was increased by approximately 2.6 kOe, which was approximately 10 % of the total coercivity. Therefore, Cu-containing low-melting-point binary alloy grain boundary addition is an effective method for optimizing the grain boundary structure of Nd-Dy-Fe-Co-B magnets, thereby improving the high-temperature stability and coercivity.