Researchers have achieved a landmark synthesis of a cerium–carbon triple bond encapsulated inside an endohedral fullerene, specifically a Ce≡CSc2 cluster within a C80 carbon cage. This work, emerging from a collaborative effort utilizing advanced crystallographic and spectroscopic techniques alongside quantum chemical analysis, breaks new ground in coordination chemistry by stabilizing lanthanide–carbon multiple bonds, which historically have been elusive due to their reactivity and structural challenges. The exceptional stability of the Ce≡C triple bond is attributed to the protective environment of the fullerene cage, which isolates and preserves the bond from external perturbations. Analytical data reveal an unprecedentedly short Ce–C bond distance of 1.969(7) Å, underscoring the strength and unique bonding character present within this organometallic complex. The research not only advances fundamental understanding of lanthanide bonding interactions but also opens avenues for exploiting such encapsulated clusters in material science and catalysis.