Dysprosium-based trimetallic nitride endohedral fullerenes (clusterfullerenes)-the Dy3N@C-2n (38 <= n <= 49) family-have been produced at overwhelming yields compared to the empty fullerenes for the first time. The Dy3N@C-2n family represents the largest clusterfullerene family explored up to now, even in comparison with the Tm3N@C-2n (38 <= n <= 44) family which was discovered very recently. A series of 10 Dy3N@C-2n clusterfullerenes (39 <= n <= 44, 1-9) have been isolated successfully and characterized by HPLC, mass spectrometry, and UV-vis-NIR spectroscopy. The study on the HPLC elution behavior reveals that there are two isomers for Dy3N@C-78 and Dy3N@C-84. Furthermore, a third isomer of Dy3N@C-80 is isolated for the first time. The optimum production conditions (Dy:C = 1: 15, NH3 pressure = 20 mbar) have been determined by investigating the effects of the Dy:C ratio and NH3 pressure on the yields of the Dy3N@C-2n clusterfullerenes. UV-vis-NIR spectroscopic study indicates that the Dy3N@C-2n clusterfullerenes with small cages (n = 3941) are large band-gap (1.38 similar to 1.51 eV) materials, while the band-gaps for those with larger cages (n = 4244) are significantly smaller (0.80 similar to 0.84 eV).