The first d1 vanadium alkylidene (neutral and cationic) was prepared in our group via an oxidatively-induced α-H abstraction route from a vanadium(III) bis-alkyl precursor. The V-C distance (1.787(3) Å) is exceedingly short with a distorted linear V-C-C angle (158.7(3)°) resulting from α-H interaction with the V(IV) center. This system is a powerful CtBu transfer reagent. For more information about this species: Basuli, F., etal. Angew. Chem. Int. Ed. 2004, 43, 3156-3159.