Reaction of TeCl4 with A1(CH3)3 in toluene affords the crystalline product [Te(CH3)3][Al(CH3)2Cl2]. The title compound crystallized in the monoclinic space group P21/n with unit cell parametersa=11.630(3),b=12.595(4),c=8.409(2) A,β=89.97(2)°, andD c =1.62 g cm−3 forZ=4. Least-squares refinement based on 1354 observed reflectionsI≥3σ (I) in the range 3.5<2Θ<45.0° led to a finalR factor of 0.046 (R w =0.067). The compound does not exist as discrete cations and anions but may be described as an organotelluronium-aluminum oligomer. The mean Te-C bond distance is 2.130(11) A while the mean Al-Cl bond distance is 2.221(4) A.