Fullerene cages are ideal hosts to encapsulate otherwise unstable metallic clusters to form endohedral metallofullerenes (EMFs). Herein, a novel TiC cluster with two titanium atoms bridged by a C-unit has been stabilized by three different fullerene cages to form TiC@(5)-C, TiC@(8)-C, and TiC@(6)-C, representing the first examples of unsupported titanium carbide clusters. Crystallographic results show that the configuration of the TiC cluster changes upon cage variation. In detail, the TiC cluster adopts a butterfly shape in TiC@(8)-C and TiC@(6)-C with Ti-C-Ti dihedral angles of 156.35 and 147.52° and Ti-Ti distances of 3.633 and 3.860 Å, respectively. In sharp contrast, a stretched planar geometry of TiC is observed in TiC@(5)-C, where a Ti-C-Ti angle of 176.87° and a long Ti-Ti distance of 5.000 Å are presented. Consistently, theoretical calculations reveal that the cluster configuration is very sensitive to the cage shape which eventually determines the electronic structures of the hybrid EMF-molecules, thus adding new insights into modern coordination chemistry.