Vanadocene (Cp2V) was reduced with potassium metal in tetrahydrofuran (THF) to give a 1:1 adduct K[Cp2V] which has been isolated as [K(THF)(Et2O)][Cp2V]. The reactions of this compound with various molecules (L) capable of functioning as ligands were investigated. They cause the liberation of KCp and the formation of several new organovanadium compounds. The products of these reactions were: [K(THF)2.5][CpVC8H12] for L = butadiene (C4H6), [K(THF)1.5][CpVC6H5P(C6H5)2] for L = P(C6H5)3,

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... (CH3)3 for L = mixture of C4H6 and P(CH3)3. Vanadocene was reacted with allyllithium to yield LiCp and [LiTMEDA][CpV(C3H5)2] (TMEDA = (CH3)2NCH2CH2N(CH3)2), which was transformed via allylbromide to CpV(C3H5)2. Structures and reactivities of these new organovanadium complexes are discussed.