A new dealkylation reaction between organophosphate esters and Salen aluminum bromide compounds has been used to prepare three new aluminum salen compounds salen(Bu-t)AlOP(O)Ph-2 (1) (salen) N,N'-ethylenebis(3,5-di-tert-butylsalicylideneimine), [(MeOH)Alsalen(Bu-t){OMePO2(O)}Alsalen(Bu-t){OMePO2(O)}Alsalen(Bu-t)]Br (2), and [salpen(Bu-t)AlO](2)[(BuO)(2)PO](2) (3) (salpen) N,N'-propylenebis(3,5-di-tert-butylsalicylideneimine). Compounds 1 center dot MeOH, 2, and 3 were characterized by single-crystal X-ray diffraction. Compound 1 is the first example of a monomeric aluminum Schiff base phosphinate. Compound 2 is a cationic Salen aluminum phosphate, and compound 3 contains an aluminophosphate ring. This work is the first example of the intentional use of an aluminum-based dealkylation reaction to form new compounds.