Reactions of oligomeric "Ca(dbbfo)(2)" and Ca-9(CH3OCH2CH2O)(18)(CH3OCH2CH2OH)(2) with Al(CH3)(3) in toluene gave tetranuclear heterobimetallic [Ca(mu-dbbfo){(mu-dbbfo)(mu-CH3)Al(CH3)(2)}](2) (71%) and polymeric Ca{(mu-CH3OCH2CH2O)(mu-CH3)Al(CH3)(2)}(2) (86%). The latter can be obtained as monomeric THF adduct Ca{(mu-CH3OCH2CH2O)Al(CH3)(3)}(2)-(THF)(2) (78%) when a mixture of solvents is used. The results, including an initial L-lactide polymerization test, are discussed in the context of calcium alkoxo cluster degradation in solution.