This paper presents methods and approaches that can be used for production of Sm-Co-Fe-Cu-Zr permanent magnets with working temperatures of up to 550 °C. It is shown that the content of Sm, Cu, and Fe significantly affects the coercivity (Hc) value at high operating temperatures. A decrease in the content of Fe, which replaces Co, and an increase in the content of Sm in Sm-Co-Fe-Cu-Zr alloys lead to a decrease inHcvalue at room temperature, but significantly increaseHcat temperatures of about 500 °C. Increasing the Cu concentration enhances theHcvalues at all operating temperatures. From analysis of the dependence of temperature coefficients of the coercivity on the concentrations of various constituent elements in this alloy, the optimum chemical composition that qualifies for high-temperature permanent magnet (HTPM) application were determined. 3D atom probe tomography analysis shows that the nanostructure of the HTPM is characterized by the formation of Sm2(Co,Fe)17(2:17) cells relatively smaller in size along with the slightly thickened Sm(Co,Cu)5(1:5) boundary phase compared to those of the high-energy permanent magnet compositions. An inhomogeneous distribution of Cu was also noticed in the 1:5 phase. At the boundary between 1:5 and 2:17 phases, an interface with lowered anisotropy constants has developed, which could be the reason for the observed high coercivity values.