To increase coercivity and thermal stability of sintered Nd–Fe–B magnets for high-temperature applications, a novel terbium sulfide powder is added into (Pr0.25Nd0.75)30.6Cu0.15FebalB1 (wt.%) basic magnets. The effects of the addition of terbium sulfide on magnetic properties, microstructure, and thermal stability of sintered Nd–Fe–B magnets are investigated. The experimental results show that by adding 3 wt.% Tb2S3, the coercivity of the magnet is remarkably increased by about 54%without a considerable reduction in remanence and maximum energy product. By means of the electron probe microanalyzer (EPMA) technology, it is observed that Tb is mainly present in the outer region of 2:14:1 matrix grains and forms a well-developed Tb-shell phase, resulting in enhancement of HA, which accounts for the coercivity enhancement. Moreover, compared with Tb2S3-free magnets, the reversible temperature coefficients of remanence (α) and coercivity (β) and the irreversible flux loss of magnetic flow (hirr) values of Tb2S3-added magnets are improved, indicating that the thermal stability of the magnets is also effectively improved.