Novel transformations of lanthanide(III) disiloxanediolates with group 13 metal trialkyls are reported. Treatment of the scandium metallacrown complex [{(Ph2SiO)2O}2{Li(DME)}2]ScCl.THF (1) with AlMe3 resulted in an Li-Al exchange reaction and the formation of the heterotrimetallic inorganic ring system [{(Ph2SiO)2O}2{Li(THF)2}AlMe2]ScCl.THF (2). The related yttrium metallacrown [{(Ph2SiO)2O}2{Li(THF)2}2]YCl.THF (3) reacts with InMe3 under the formation of the heterobimetallic Y/In disiloxanediolate complex [{(Ph2SiO)2O}2{InMe2(OMe)}2InMe2]Y (4). In the latter, two monomeric Me2InOMe ligands are stabilized through coordination to yttrium.