Metal nitride clusterfullerenes (NCFs) have significant applications in molecular electronics, biomedical imaging, and nonlinear optical devices due to their unique structures. However, their wide applications are limited by the production quantity. In this work, the yields of metal nitride clusterfullerenes M 3 N@C 80 (M=Y, Sc, Gd) were greatly enhanced by utilizing zirconium nitride (ZrN) as an efficient nitrogen source for the arc-discharge method. Compared with the traditional synthetic route using N 2 gas as nitrogen source, the ZrN inside graphite tube can be vaporized simultaneously with metal and graphite, and then afford the high concentration of nitrogen atoms in the arc region, which will promote the formation of metal nitride clusterfullerenes finally. The ZrN can promote the yields of Y 3 N@C 80 , Sc 3 N@C 80 and Gd 3 N@C 80 , revealing the universal applicability of ZrN as a highly efficient nitrogen source. Specifically, the yield of Sc 3 N@C 80 was greatly improved when adding ZrN, and it shows over double yield compared to traditional synthetic route using N 2 gas. In addition, ZrN can also enhance the yields of paramagnetic azametallofullerene M 2 @C 79 N due to the high concentration of nitrogen atoms in the arc region. This new method enhances the production quantity of metal nitride clusterfullerenes and azametallofullerenes, and it will greatly promote the research and application of these molecular carbon materials. metal nitride clusterfullerenes, zirconium nitride, nitrogen source, high yield, arc-discharge method