Zirconium dialkyl complexes of the general formula fc(NPiPr(2))(2)ZrR, (where fc = 1,11-ferrocenyl, R = CH3, CH2Ph, CH2Bu,Bu) have been synthesized and characterized via the addition of alkyl lithium or potassium benzyl derivatives to the dichloride complex fc(NP'Pr-2),ZrC1,(THF). Addition of 2,6-dimethylphenylisocyanide to these alkyl derivatives generates the corresponding mono iminoacyl alkyl zirconium complexes. On thermolysis, the iminoacyl moiety containing a benzyl substituent undergoes rearrangement to yield a new complex that contains an alkene-amido fragment. Mechanistic studies point to a 1,2 hydrogen shift as the rate -determining step.