Titanium carbide anionic clusters have been generated and analyzed by time-of-flight mass spectrometry. Our experiments successfully reproduced all the reported magic numbers in the lower mass range (<1200 amu), i.e. Ti 3C 8-, Ti 6C 13-, Ti 7C 13-, Ti 9C 15-, Ti 13C 22-, and Ti 14C 24- [Phys. Rev. Lett. 78 (1997) 2983; J. Am. Chem. Soc. 120 (1998) 6556]. In the higher mass range up to 1800 amu, new magic numbers at Ti 15C 26-, Ti 20C 33-/Ti 20C 34-, and Ti 25C 42- are found, which cannot be understood by any of the previously proposed structural growth models. A staggered layer-by-layer growth pathway based on Ti 5C 8 subunits is introduced. Density functional calculations show high stabilities of the constructed structures.