Uranyl complexes of a bis(methylterephthalamide) ligand (LH4) have been synthesized and characterized by X-ray crystallography. The structure is an unexpected [Me4N]8[L(UO2)]4 tetramer, formed via coordination of the two MeTAM units of L to two uranyl moieties. Addition of KOH to the tetramer gave the corresponding monomeric uranyl methoxide species [Me4N]K2[LUO2(OMe)].