Intergranular addition using heavy rare earth (HRE) Dy/Tb containing alloys has been an effective way to modulate the microstructure and chemical distribution towards fabricating high-coercivity Nd-Fe-B sintered magnets. In this work, (Pr20Nd80)60Tb15Cu15Ga10 (at%) intergranular alloy powders were designed and introduced with dual purposes of forming Tb-rich matrix shell and antiferromagnetic RE6Fe13Ga grain boundary phase (GBP). With 3 wt% (Pr20Nd80)60Tb15Cu15Ga10 addition, the coercivity Hcj is significantly increased from 11.1 kOe to 17.9 kOe, accompanied with a high utilization efficiency of Tb (11.8 kOe/%) and a superior temperature coefficient of coercivity β(−0.531%/K). Microstructural analysis suggests that the improved wettability of grain boundary by (Pr20Nd80)60Tb15Cu15Ga10 addition is beneficial to form the Tb-rich matrix shell and antiferromagnetic RE6Fe13Ga GBP throughout the bulk magnets. Micromagnetic simulation is implemented to study the effect of formed ferromagnetic/antiferromagnetic GBP and Tb-rich matrix shell on the magnetization reversal process. Results show that the synergy of Tb-rich shell surrounding Nd/Pr-rich core and antiferromagnetic Nd/Pr-rich RE6Fe13Ga GBP is an effective way to promote the coercivity with high utilization efficiency of HRE Tb.