A dealkylsilylation reaction between alumazene [2,6-(i-Pr)(2)C(6)H(3)NAlMe](3) (1) and tris(trimethylsilyl) ester of phosphoric acid (2) in a 1:3 molar ratio provides the heteroadamantane molecule (MeAl)[2,6-(i-Pr)(2)C(6)H(3)N](3)[Al[OP(OSiMe(3))(3)]](2)(O(3)POSiMe(3)) (3). Compound 3 was characterized by analytical and spectroscopic methods, and its molecular structure was established by a single-crystal X-ray diffraction experiment. Moreover, trialkyl and triaryl phosphates and dialkyl phosphonates react with 1 at elevated temperature to afford an intractable mixture of products. The reaction of phosphonic acids with 1 proceeds under decomposition to yield 2,6-diisopropylaniline and aluminophosphonates.