Novel mono- and bimetallic scorpionate aluminum compounds have been designed and characterized by spectroscopic methods. These organometallics complexes, in combination with tetrabutylammonium bromide as cocatalyst, displayed good catalytic activity for the cycloaddition of styrene oxide and CO under ambient conditions. Among the compounds tested, monometallic complex 3 featuring diethylamino groups showed the highest catalytic activity. This catalytic system catalyzed the formation of cyclic carbonate products from their corresponding epoxides at room temperature and 1 bar of CO pressure in the absence of a solvent in good yields and excellent selectivities.