The bulky chelating dianion Me2Si(NDipp-)2 has been used to synthesize [{Me2Si(NDipp)2}ZrCl2(THF)2] (Dipp = 2,6-diisopropylphenyl). Reaction of Al2Me6 and [{Me2Si(NDipp)2}ZrCl2(THF)2] affords the unusual ionic complex [Me2Al(THF)2]+[{Me2Si(NDipp)2}2Zr2Cl5]-.