Anionic donor-functionalized NHC (N-heterocyclic carbene) complexes of Al are rare. We report one such case here, a NHC-aryloxido AlMe2 complex [Al(L)Me2] (2), following a stepwise synthesis from the proligand [HO-4,6-tBu2-C6H2-2-CH2{CH(NCH=CHNAr)}]Br...